Light‐Driven Active Proton Transport through Photoacid‐ and Photobase‐Doped Janus Graphene Oxide Membranes

Biological electrogenic systems use protein‐based ionic pumps to move salt ions uphill across a cell membrane to accumulate an ion concentration gradient from the equilibrium physiological environment. Toward high‐performance and robust artificial electric organs, attaining an antigradient ion transport mode by fully abiotic materials remains a great challenge. Herein, a light‐driven proton pump transport phenomenon through a Janus graphene oxide membrane (JGOM) is reported. The JGOM is fabricated by sequential deposition of graphene oxide (GO) nanosheets modified with photobase (BOH) and photoacid (HA) molecules. Upon ultraviolet light illumination, the generation of a net protonic photocurrent through the JGOM, from the HA‐GO to the BOH‐GO side, is observed. The directional proton flow can thus establish a transmembrane proton concentration gradient of up to 0.8 pH units mm^?2 membrane area at a proton transport rate of 3.0 mol h^?1 m^?2. Against a concentration gradient, antigradient proton transport can be achieved. The working principle is explained in terms of asymmetric surface charge polarization on HA‐GO and BOH‐GO multilayers triggered by photoisomerization reactions, and the consequent intramembrane proton concentration gradient. The implementation of membrane‐scale light‐harvesting 2D nanofluidic system that mimics the charge process of the bioelectric organs makes a straightforward step toward artificial electrogenic and photosynthetic applications.     

Fabrication of Millimeter‐Long Carbon Tubular Nanostructures Using the Self‐Rolling Process Inherent in Elastic Protein Layers

Millimeter‐long conducting fibers can be fabricated from carbon nanomaterials via a simple method involving the release of a prestrained protein layer. This study shows how a self‐rolling process initiated by polymerization of a micropatterned layer of fibronectin (FN) results in the production of carbon nanomaterial‐based microtubular fibers. The process begins with deposition of carbon nanotube (CNT) or graphene oxide (GO) particles on the FN layer. Before polymerization, particles are discrete and nonconducting, but after polymerization the carbon materials become entangled to form an interconnected conducting network clad by FN. Selective removal of FN using high‐temperature combustion yields freestanding CNT or reduced GO microtubular fibers. The properties of these fibers are characterized using atomic force microscopy and Raman spectroscopy. The data suggest that this method may provide a ready route to rapid design and fabrication of aligned biohybrid nanomaterials potentially useful for future electronic applications.     

Hierarchical 3D All‐Carbon Composite Structure Modified with N‐Doped Graphene Quantum Dots for High‐Performance Flexible Supercapacitors

Flexible supercapacitors have shown enormous potential for portable electronic devices. Herein, hierarchical 3D all‐carbon electrode materials are prepared by assembling N‐doped graphene quantum dots (N‐GQDs) on carbonized MOF materials (cZIF‐8) interweaved with carbon nanotubes (CNTs) for flexible all‐solid‐state supercapacitors. In this ternary electrode, cZIF‐8 provides a large accessible surface area, CNTs act as the electrical conductive network, and N‐GQDs serve as highly pseudocapactive materials. Due to the synergistic effect and hierarchical assembly of these components, N‐GQD@cZIF‐8/CNT electrodes exhibit a high specific capacitance of 540 F g^?1 at 0.5 A g^?1 in a 1 m H₂SO₄ electrolyte and excellent cycle stability with 90.9% capacity retention over 8000 cycles. The assembled supercapacitor possesses an energy density of 18.75 Wh kg^?1 with a power density of 108.7 W kg^?1. Meanwhile, three supercapacitors connected in series can power light‐emitting diodes for 20 min. All‐solid‐state N‐GQD@cZIF‐8/CNT flexible supercapacitor exhibits an energy density of 14 Wh kg^?1 with a power density of 89.3 W kg^?1, while the capacitance retention after 5000 cycles reaches 82%. This work provides an effective way to construct novel electrode materials with high energy storage density as well as good cycling performance and power density for high‐performance energy storage devices via the rational design.     

A Cut‐and‐Paste Approach to 3D Graphene‐Oxide‐Based Architectures

Properly cut sheets can be converted into complex 3D structures by three basic operations including folding, bending, and pasting to render new functions. Folding and bending are extensively employed in crumpling, origami, and pop‐up fabrications for 3D structures. Pasting joins different parts of a material together, and can create new geometries that are fundamentally unattainable by folding and bending. However, it has been much less explored, likely due to limited choice of weldable thin film materials and residue‐free glues. Here it is shown that graphene oxide (GO) paper is one such suitable material. Stacked GO sheets can be readily loosened up and even redispersed in water, which upon drying, restack to form solid structures. Therefore, water can be utilized to heal local damage, glue separated pieces, and release internal stress in bent GO papers to fix their shapes. Complex and dynamic 3D GO architectures can thus be fabricated by a cut‐and‐paste approach, which is also applicable to GO‐based hybrid with carbon nanotubes or clay sheets.     

Micrometer‐Thick Graphene Oxide–Layered Double Hydroxide Nacre‐Inspired Coatings and Their Properties

Robust, functional, and flame retardant coatings are attractive in various fields such as building construction, food packaging, electronics encapsulation, and so on. Here, strong, colorful, and fire‐retardant micrometer‐thick hybrid coatings are reported, which can be constructed via an enhanced layer‐by‐layer assembly of graphene oxide (GO) nanosheets and layered double hydroxide (LDH) nanoplatelets. The fabricated GO–LDH hybrid coatings show uniform nacre‐like layered structures that endow them good mechanic properties with Young's modulus of ≈18 GPa and hardness of ≈0.68 GPa. In addition, the GO–LDH hybrid coatings exhibit nacre‐like iridescence and attractive flame retardancy as well due to their well‐defined 2D microstructures. This kind of nacre‐inspired GO–LDH hybrid thick coatings will be applied in various fields in future due to their high strength and multifunctionalities.     

Synthetic Multifunctional Graphene Composites with Reshaping and Self‐Healing Features via a Facile Biomineralization‐Inspired Process

Since graphene is a type of 2D carbon material with excellent mechanical, electrical, thermal, and optical properties, the efficient preparation of graphene macroscopic assemblies is significant in the potentially large‐scale application of graphene sheets. Conventional preparation methods of graphene macroscopic assemblies need strict conditions, and, once formed, the assemblies cannot be edited, reshaped, or recycled. Herein, inspired by the biomineralization process, a feasible approach of shapeable, multimanipulatable, and recyclable gel‐like composite consisting of graphene oxide/poly(acrylic acid)/amorphous calcium carbonate (GO‐PAA‐ACC) is designed. This GO‐PAA‐ACC material can be facilely synthesized at room temperature with a cross‐linking network structure formed during the preparation process. Remarkably, it is stretchable, malleable, self‐healable, and easy to process in the wet state, but tough and rigid in the dried state. In addition, these two states can be readily switched by adjusting the water content, which shows recyclability and can be used for 3D printing to form varied architectures. Furthermore, GO‐PAA‐ACC can be functionalized or processed to meet a variety of specific application requirements (e.g., energy‐storage, actuators). The preparation method of GO‐PAA‐ACC composite in this work also provides a novel strategy for the versatile macroscopic assembly of other materials, which is low‐cost, efficient, and convenient for broad application.     

Sub‐10 nm Ag Nanoparticles/Graphene Oxide: Controllable Synthesis,Size‐Dependent and Extremely Ultrahigh Catalytic Activity

While tremendous advancements in Ag nanoparticle (AgNP)‐based materials have been made, the development of a facile protocol for preparing sub‐10 nm AgNPs with controllable size and ultrahigh performance remains a formidable challenge. It is shown that AgNPs/graphene oxide (AgNPs/GO) bearing 2.5, 4.3, and 6.2 nm AgNPs (2.5‐AgNPs/GO, 4.3‐AgNPs/GO, and 6.2‐AgNPs/GO, respectively) could be fabricated via light‐induced synthesis. Their catalytic activity toward 4‐nitrophenol (4‐NP) reduction, which is a “gold standard” for evaluating the performance of noble metal–based catalysts, is studied. When normalized by mole and area, the activity exhibits an order of 4.3‐AgNPs/GO > 6.2‐AgNPs/GO > 2.5‐AgNPs/GO and 6.2‐AgNPs/GO > 4.3‐AgNPs/GO > 2.5‐AgNPs/GO, respectively. This trend is a result of GO‐induced electron concentration reduction with decreasing AgNP size. Significantly, under similar conditions, the activity of 4.3‐AgNPs/GO is substantially superior to that of numerous state‐of‐the‐art noble metal–based catalysts. The ultrafine size of the AgNPs and their surface accommodation on the unobstructed 2D GO scaffolds without capping reagents/covers, which make the abundantly exposed catalytically active sites highly accessible to substrate molecules, play an important role in their extremely ultrahigh performance. This work paves a new avenue for high‐performance AgNP‐based materials, and by taking 4‐NP reduction as a proof‐of‐concept, provides new scientific insights into the rational design of surface‐based advanced materials.     

Self‐Assembly of Graphene Oxide at Interfaces

Due to its amphiphilic property, graphene oxide (GO) can achieve a variety of nanostructures with different morphologies (for example membranes, hydrogel, crumpled particles, hollow spheres, sack‐cargo particles, Pickering emulsions, and so on) by self‐assembly. The self‐assembly is mostly derived from the self‐concentration of GO sheets at various interfaces, including liquid‐air, liquid‐liquid and liquid‐solid interfaces. This paper gives a comprehensive review of these assembly phenomena of GO at the three types of interfaces, the derived interfacial self‐assembly techniques, and the as‐obtained assembled materials and their properties. The interfacial self‐assembly of GO, enabled by its fantastic features including the amphiphilicity, the negatively charged nature, abundant oxygen‐containing groups and two‐dimensional flexibility, is highlighted as an easy and well‐controlled strategy for the design and preparation of functionalized carbon materials, and the use of self‐assembly for uniform hybridization is addressed for preparing hybrid carbon materials with various functions. A number of new exciting and potential applications are also presented for the assembled GO‐based materials. This contribution concludes with some personal perspectives on future challenges before interfacial self‐assembly may become a major strategy for the application‐targeted design and preparation of functionalized carbon materials.     

Porous TiNi Biomaterial by Self‐Propagating High‐Temperature Synthesis

Porous TiNi shape‐memory alloy (TiNi SMA) bodies with controlled pore structure were produced from the (Ti+Ni) powder mixture by self‐propagating high‐temperature synthesis (SHS) method. The effect of processing variables such as the kind of starting powders, ignition temperature and preheating schedule on the behavior of combustion wave propagation, the formation of phases and pore structure was investigated. The relationship between pore structure and mechanical properties was also investigated. An in vivo test was performed to evaluate bone tissue response and histocompatibility of porous TiNi SMA using 15 New Zealand white rabbits. No apparent adverse reactions such as inflammation and foreign body reaction were noted on or around all implanted porous TiNi SMA blocks. Bone ingrowth was found in the pore space of all implanted blocks.     

Large Photothermal Effect in Sub‐40 nm h‐BN Nanostructures Patterned Via High‐Resolution Ion Beam

The controlled nanoscale patterning of 2D materials is a promising approach for engineering the optoelectronic, thermal, and mechanical properties of these materials to achieve novel functionalities and devices. Herein, high‐resolution patterning of hexagonal boron nitride (h‐BN) is demonstrated via both helium and neon ion beams and an optimal dosage range for both ions that serve as a baseline for insulating 2D materials is identified. Through this nanofabrication approach, a grating with a 35 nm pitch, individual structure sizes down to 20 nm, and additional nanostructures created by patterning crystal step edges are demonstrated. Raman spectroscopy is used to study the defects induced by the ion beam patterning and is correlated to scanning probe microscopy. Photothermal and scanning near‐field optical microscopy measure the resulting near‐field absorption and scattering of the nanostructures. These measurements reveal a large photothermal expansion of nanostructured h‐BN that is dependent on the height to width aspect ratio of the nanostructures. This effect is attributed to the large anisotropy of the thermal expansion coefficients of h‐BN and the nanostructuring implemented. The photothermal expansion should be present in other van der Waals materials with large anisotropy and can lead to applications such as nanomechanical switches driven by light.     

2D Layered Graphene Oxide Films Integrated with Micro‐Ring Resonators for Enhanced Nonlinear Optics

Layered 2D graphene oxide (GO) films are integrated with micro‐ring resonators (MRRs) to experimentally demonstrate enhanced nonlinear optics. Both uniformly coated (1?5 layers) and patterned (10?50 layers) GO films are integrated on complementary‐metal‐oxide‐semiconductor (CMOS)‐compatible doped silica MRRs using a large‐area, transfer‐free, layer‐by‐layer GO coating method with precise control of the film thickness. The patterned devices further employ photolithography and lift‐off processes to enable precise control of the film placement and coating length. Four‐wave‐mixing (FWM) measurements for different pump powers and resonant wavelengths show a significant improvement in efficiency of ≈7.6 dB for a uniformly coated device with 1 GO layer and ≈10.3 dB for a patterned device with 50 GO layers. The measurements agree well with theory, with the enhancement in FWM efficiency resulting from the high Kerr nonlinearity and low loss of the GO films combined with the strong light–matter interaction within the MRRs. The dependence of GO's third‐order nonlinearity on layer number and pump power is also extracted from the FWM measurements, revealing interesting physical insights about the evolution of the GO films from 2D monolayers to quasi bulk‐like behavior. These results confirm the high nonlinear optical performance of integrated photonic resonators incorporated with 2D layered GO films.     

Template‐Mediated Assembly of DNA into Microcapsules for Immunological Modulation

There is a need for effective vaccine delivery systems and vaccine adjuvants without extraneous excipients that can compromise or minimize their efficacy. Vaccine adjuvants cytosine–phosphate–guanosine oligodeoxynucleotides (CpG ODNs) can effectively activate immune responses to secrete cytokines. However, CpG ODNs are not stable in serum due to enzymatic cleavage and are difficult to transport through cell membranes. Herein, DNA microcapsules made of CpG ODNs arranged into 3D nanostructures are developed to improve the serum stability and immunostimulatory effect of CpG. The DNA microcapsules allow encapsulation and co‐delivery of cargoes, including glycogen. The DNA capsules, with >4 million copies of CpG motifs per capsule, are internalized in cells and accumulate in endosomes, where the Toll‐like receptor 9 is engaged by CpG. The capsules induce up to 10‐fold and 20‐fold increases in tumor necrosis factor (TNF)‐α and interleukin (IL)‐6 secretion, respectively, in RAW264.7 cells compared with CpG ODNs. Furthermore, the microcapsules stimulate TNF‐α and IL‐6 secretion in a concentration‐ and time‐dependent manner. The immunostimulatory activity of the capsules correlates to their intracellular trafficking, endosomal confinement, and degradation, assessed by confocal and super‐resolution microscopy. These DNA capsules can serve as both adjuvants to stimulate an immune reaction and vehicles to encapsulate vaccine peptides/genes to achieve synergistic immune effects.     

Near‐Infrared Activated Black Phosphorus as a Nontoxic Photo‐Oxidant for Alzheimer's Amyloid‑β Peptide

The inhibition of amyloid‐β (Aβ) aggregation by photo‐oxygenation has become an effective way of treating Alzheimer's disease (AD). New near‐infrared (NIR) activated treatment agents, which not only possess high photo‐oxygenation efficiency, but also show low biotoxicity, are urgently needed. Herein, for the first time, it is demonstrated that NIR activated black phosphorus (BP) could serve as an effective nontoxic photo‐oxidant for amyloid?β peptide in vitro and in vivo. The nanoplatform BP@BTA (BTA: one of thioflavin‐T derivatives) possesses high affinity to the Aβ peptide due to specific amyloid selectivity of BTA. Importantly, under NIR light, BP@BTA can significantly generate a high quantum yield of singlet oxygen (¹O₂) to oxygenate Aβ, thereby resulting in inhibiting the aggregation and attenuating Aβ‐induced cytotoxicity. In addition, BP could finally degrade into nontoxic phosphate, which guarantees the biosafety. Using transgenic Caenorhabditis elegans CL2006 as AD model, the results demonstrate that the ¹O₂‐generation system could dramatically promote life‐span extension of CL2006 strain by decreasing the neurotoxicity of Aβ.     

Self‐Assembly of Enzyme‐Like Nanofibrous G‐Molecular Hydrogel for Printed Flexible Electrochemical Sensors

Conducting hydrogels provide great potential for creating designer shape‐morphing architectures for biomedical applications owing to their unique solid–liquid interface and ease of processability. Here, a novel nanofibrous hydrogel with significant enzyme‐like activity that can be used as “ink” to print flexible electrochemical devices is developed. The nanofibrous hydrogel is self‐assembled from guanosine (G) and KB(OH)₄ with simultaneous incorporation of hemin into the G‐quartet scaffold, giving rise to significant enzyme‐like activity. The rapid switching between the sol and gel states responsive to shear stress enables free‐form fabrication of different patterns. Furthermore, the replication of the G‐quartet wires into a conductive matrix by in situ catalytic deposition of polyaniline on nanofibers is demonstrated, which can be directly printed into a flexible electrochemical electrode. By loading glucose oxidase into this novel hydrogel, a flexible glucose biosensor is developed. This study sheds new light on developing artificial enzymes with new functionalities and on fabrication of flexible bioelectronics.     

Controlling Long‐Distance Photoactuation with Protein Additives

Long‐distance wireless actuation indicates precise remote control over materials, sensors, and devices that are widely utilized in biomedical, defence, disaster relief, deep ocean, and outer space applications to replace human work. Unlike radio frequency (RF) control, which has low tolerance toward electromagnetic interference (EMI), light control represents a promising method to overcome EMI. Nonetheless, long‐distance light‐controlled wireless actuation able to compete with RF control has not been achieved until now due to the lack of highly light‐sensitive actuator designs. Here, it is demonstrate that amyloid‐like protein aggregates can organize photomodule single‐layer reduced graphene oxide (rGO) into a well‐defined multilayer stack to display long‐distance photoactuation. The amyloid‐like proteinaceous component docks the rGO layers together to form a hybrid film, which can reliably adhere onto various material surfaces with robust interfacial adhesion. The sensitive photothermal effect and a fast bending in 1 s to switch a circuit are achieved after forming the film on a plastic substrate and irradiating the bilayer film with a blue laser from 100 m away. A photoactuation distance of 50 km can be further extrapolated based on a commercial high‐power laser. This study reveals the great potential of amyloid‐like aggregates in remote light control of robots and devices.     

Cyanine‐Anchored Silica Nanochannels for Light‐Driven Synergistic Thermo‐Chemotherapy

Smart nanoparticles are increasingly important in a variety of applications such as cancer therapy. However, it is still a major challenge to develop light‐responsive nanoparticles that can maximize the potency of synergistic thermo‐chemotherapy under light irradiation. Here, spatially confined cyanine‐anchored silica nanochannels loaded with chemotherapeutic doxorubicin (CS‐DOX‐NCs) for light‐driven synergistic cancer therapy are introduced. CS‐DOX‐NCs possess a J‐type aggregation conformation of cyanine dye within the nanochannels and encapsulate doxorubicin through the π–π interaction with cyanine dye. Under near‐infrared light irradiation, CS‐DOX‐NCs produce the enhanced photothermal conversion efficiency through the maximized nonradiative transition of J‐type Cypate aggregates, trigger the light‐driven drug release through the destabilization of temperature‐sensitive π–π interaction, and generate the effective intracellular translocation of doxorubicin from the lysosomes to cytoplasma through reactive oxygen species‐mediated lysosomal disruption, thereby causing the potent in vivo hyperthermia and intracellular trafficking of drug into cytoplasma at tumors. Moreover, CS‐DOX‐NCs possess good resistance to photobleaching and preferable tumor accumulation, facilitating severe photoinduced cell damage, and subsequent synergy between photothermal and chemotherapeutic therapy with tumor ablation. These findings provide new insights of light‐driven nanoparticles for synergistic cancer therapy.     

A Flexible Caterpillar‐Like Gold Nanoparticle Assemblies with Ultrasmall Nanogaps for Enhanced Dual‐Modal Imaging and Photothermal Therapy

Gold nanoparticle (AuNP) assemblies (GNAs) have attracted attention since enhanced coupling plasmonic resonance (CPR) emerged in the nanogap between coupling AuNPs. For one dimensional GNAs (1D‐GNAs), most CPR from the nanogaps could be easily activated by electromagnetic waves and generate drastically enhanced CPR because the nanogaps between coupling AuNPs are linearly distributed in the 1D‐GNAs. The reported studies focus on the synthesis of 1D‐GNAs and fundamental exploration of CPR. There are still problems which impede further applications in nanomedicine, such as big size (>500 nm), poor water solubility, and/or poor stability. In this study, a kind of 1D flexible caterpillar‐like GNAs (CL‐GNAs) with ultrasmall nanogaps, good water solubility, and good stability is developed. The CL‐GNAs have a flexible structure that can randomly move to change their morphology, which is rarely reported. Numerous ultrasmall nanogaps (<1 nm) are linearly distributed along the structure of CL‐GNAs and generate enhanced CPR. The toxicity assessments in vitro and vivo respectively demonstrate that CL‐GNAs have a low cytotoxicity and good biocompatibility. The CL‐GNAs can be used as an efficient photothermal agent for photothermal therapy, a probe for Raman imaging and photothermal imaging.     

Sulfur and Nitrogen Co‐Doped Graphene for Metal‐Free Catalytic Oxidation Reactions

Sulfur and nitrogen co‐doped reduced graphene oxide (rGO) is synthesized by a facile method and demonstrated remarkably enhanced activities in metal‐free activation of peroxymonosulfate (PMS) for catalytic oxidation of phenol. Based on first‐order kinetic model, S–N co‐doped rGO (SNG) presents an apparent reaction rate constant of 0.043 ± 0.002 min^?1, which is 86.6, 22.8, 19.7, and 4.5‐fold as high as that over graphene oxide (GO), rGO, S‐doped rGO (S‐rGO), and N‐doped rGO (N‐rGO), respectively. A variety of characterization techniques and density functional theory calculations are employed to investigate the synergistic effect of sulfur and nitrogen co‐doping. Co‐doping of rGO at an optimal sulfur loading can effectively break the inertness of carbon systems, activate the sp²‐hybridized carbon lattice and facilitate the electron transfer from covalent graphene sheets for PMS activation. Moreover, both electron paramagnetic resonance (EPR) spectroscopy and classical quenching tests are employed to investigate the generation and evolution of reactive radicals on the SNG sample for phenol catalytic oxidation. This study presents a novel metal‐free catalyst for green remediation of organic pollutants in water.     

Biodegradable Nanocomposite with Dual Cell‐Tissue Penetration for Deep Tumor Chemo‐Phototherapy

Chemo‐phototherapy, as a promising cancer combination therapy strategy, has attracted widespread attention. However, the complex tumor microenvironment restricts the penetration depth of chemo‐phototherapy agents in the tumor region. Here, biodegradable amphiphilic gelatin (AG) wrapped nanocomposite (PRDCuS@AG) composed of doxorubicin and copper sulfide (CuS)‐loaded dendrimer is designed for deep tumor chemo‐phototherapy. PR in PRDCuS@AG represents arginine‐conjugated polyamidoamine dendrimer. PRDCuS@AG can rapidly biodegrade into PRDCuS by matrix metalloproteinases under near‐infrared light irradiation. The resulted PRDCuS harbors dual cell‐tissue penetration ability, which can effectively penetrate deep into the tumor tissue. In particular, PRDCuS@AG achieves photoacoustic imaging‐guided synergistic chemo‐phototherapy with 97% of tumor inhibition rate. Moreover, PRDCuS@AG can further degrade into 3 nm ultrasmall CuS, which can be eliminated from the body after treatment to avoid side effects. This strategy provides an insight that the development of chemo‐phototherapy agents with high penetration ability to overcome the limitation of current deep tumor therapy.     

Polyethylene Glycol and Polyethylenimine Dual‐Functionalized Nano‐Graphene Oxide for Photothermally Enhanced Gene Delivery

Graphene oxide (GO) has been extensively explored in nanomedicine for its excellent physiochemical, electrical, and optical properties. Here, polyethylene glycol (PEG) and polyethylenimine (PEI) are covalently conjugated to GO via amide bonds, obtaining a physiologically stable dual‐polymer‐functionalized nano‐GO conjugate (NGO‐PEG‐PEI) with ultra‐small size. Compared with free PEI and the GO‐PEI conjugate without PEGylation, NGO‐PEG‐PEI shows superior gene transfection efficiency without serum interference, as well as reduced cytotoxicity. Utilizing the NIR optical absorbance of NGO, the cellular uptake of NGO‐PEG‐PEI is shown to be enhanced under a low power NIR laser irradiation, owing to the mild photothermal heating that increases the cell membrane permeability without significantly damaging cells. As the results, remarkably enhanced plasmid DNA transfection efficiencies induced by the NIR laser are achieved using NGO‐PEG‐PEI as the light‐responsive gene carrier. More importantly, it is shown that our NGO‐PEG‐PEI is able to deliver small interfering RNA (siRNA) into cells under the control of NIR light, resulting in obvious down‐regulation of the target gene, Polo‐like kinase 1 (Plk1), in the presence of laser irradiation. This study is the first to use photothermally enhanced intracellular trafficking of nanocarriers for light‐controllable gene delivery. This work also encourages further explorations of functionalized nano‐GO as a photocontrollable nanovector for combined photothermal and gene therapies.