Five different grades of maleic anhydride polypropylene (MAPP) having different molecular weight and acid value (AV) were used as coupler in PP-nanocrystalline cellulose (NCC) composites. The main objective was to study the effect of MAPP structure (Mw, AV) and filler/coupler (F/C) ratio on mechanical properties in order to find optimum mechanical properties in tension, flexion, and impact. Results showed that both Mw and AV have direct effect on mechanical properties and a balance between both must be achieved to get the best performance. However, regardless of MAPP structure, optimum improvement was obtained for F/C 5 7.5/1. Shear rheological data showed that at high MAPP content, MAPP acts as lubricant. DSC and AFM analysis showed small reduction in the size of PP crystals in the presence of NCC. Rheological data under large amplitude oscillatory shear showed that the nanocomposites used here are under percolation. Using these analyses, possible reinforcement mechanisms were investigated. V C 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015, 132, 42438.