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Biocomposites with tunable properties were successfully prepared through ionic assembly between anionic carboxymethyl cellulose (CMC) and cationic copolymers (quaternized poly( l -lactide)-block-poly N , N -dimethylamino-2-ethyl methacrylate) (PLA- b -PDMAEMA). The quaternized PDMAEMA segment not only works as a compatibilizer between hydrophilic CMC and hydrophobic PLA, but also acts as a lubricant between these two rigid biopolymers. The 1 H NMR (nuclear magnetic resonance) spectra demonstrated successful synthesis of PLA- b -PDMAEMA with controlled molecular weight of PDMAEMA segment. The results from scanning electronic microscopy (SEM) and Fourier transform infrared spectrometry (FTIR) verified the interaction between quaternized copolymer micelles and anionic CMC networks. The resultant biocomposite could form a transparent and uniform film after casting. Both storage moduli and maximum degradation temperature of PLA/CMC composites were increased with the reduction of molecular weight of PDMAEMA segments. It suggests that the properties of biocomposite materials can be tailored by adjusting the chain length of inclusive PDMAEMA segment. [ABSTRACT FROM AUTHOR]