In order to achieve the effective interface bonding between biomass microfiller and commodity plastics, consecutive copolymerization of hydrophilic acrylic acid (AA) and hydrophobic butyl acrylate (BA) using vapor-phase assisted surface polymerization (VASP) technology was applied to prepare microcomposites consisting of cellulose microcrystal (ClC) and polypropylene (PP). After the copolymerization by VASP, ClC surfaces were covered by accumulated polymers: P(AA-co-BA) including block-type copolymer and homopolymers of 6.2-25.3 wt % versus ClC. Although structures of the products were unspecified, it was expected to be mixtures of block copolymers and homopolymers. Subsequently prepared P(AA-co-BA) on ClC/PP (5/95 wt/wt) composites expressed a superior mechanical toughness, which had increased threefold when compared to intact ClC/PP composite. This increase in toughness was mainly based on an increase in elongation rate, reflecting improvement of the adhesion strength at the interface between ClC surface and PP. The trace amounts: 0.31 wt % of accumulated P(AA-co-BA) on ClC surface must function as an effective adhesive/compatibilizer at the interface.