Abstract: | This study systematically investigates the polymer–carbon nanotube (CNT) interaction when the interphase is tailored. Maleic anhydride‐grafted‐polypropylene (MA‐g‐PP) or polypropylene (PP) was noncovalently coated onto acid functionalized multiwall nanotube (f‐MWNT) through solution mixing. These coated f‐MWNTs were melt microcompounded with neat PP to form PP/f‐MWNT nanocomposites. The effects of functional groups and the thin layer of solution processed polymers, namely, MA‐g‐PP or PP, at the PP/f‐MWNT interface on crystallization and on melting behavior of matrix PP were investigated. The results were compared with a pristine MWNT (p‐MWNT) incorporated system. It was shown that PP coated CNTs can serve as a strong nucleating agent for templated polymer crystal growth. Unlike other PP nanocomposites in the literature, a relatively high shift of 7°C in melting peak maximum (Tp), along with a sharp melt endotherm was achieved with the addition of 0.3 wt% f‐MWNT via PP/f‐MWNT master batch. This indicates refinement of matrix PP crystalline region due to the tailored f‐MWNT surface chemistry. With a designed self‐seeding and templated crystal growth approach, columnar crystalline interphases were found surrounding MWNT which melted at 10.5°C higher temperature than neat PP crystallized without undergoing the same heat treatment protocol. POLYM. ENG. SCI., 59:1570–1584 2019. © 2019 Society of Plastics Engineers |