This study aimed to fabricate polyelectrolyte complexes from water-soluble poly(ethylene glycol) methyl ether-grafted chitosan (mPEG-g-CTS) and alginate (ALG) in the absence of acetic acid. The complexes formed fibrous network macrogels when mPEG-g-CTS with short mPEG chains (mPEG750-g-CTS and mPEG2000-g-CTS) and mPEG-g-CTS:ALG weight ratios in the range from 1:0.14 to 1:1 were used. The macrogels at a weight ratio of mPEG-g-CTS:ALG of 1:1 possessed the highest elasticity with electrophoretic mobility close to 0 m·V·s. Water uptake of the sponge-like lyophilized macrogels decreased with increasing ALG content, mPEG chain length, and degree of substitution of mPEG-g-CTS. In contrast, the polyelectrolyte complexes prepared using long mPEG chains of mPEG-g-CTS (mPEG5000-g-CTS) formed spherical nanoparticles (70-90 nm) and showed highly negative electrophoretic mobility (< -3.20 × 10 m·V·s). The obtained mPEG-g-CTS/ALG polyelectrolyte complex hydrogels and nanoparticles have the potential to be applied as carriers for functional food additives, drugs, and bioactive compounds.
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