This study presents a facile, green, and sustainable method for the integrated production of chitin nanocrystals (ChNCs) and nanofibers (ChNFs) from shrimp shell chitin using recyclable maleic acid and microwave irradiation. Maleic acid, a mild organic acid, is employed for hydrolysis and functionalization, with 88.5% recovery for reuse, contributing to the sustainability of the process. Optimal production conditions, determined using response surface methodology (RSM), were an 85% acid concentration, 26.63 min of reaction time, and 315.41 W microwave power, yielding 26.28% ChNCs and 64.04% ChNFs. Transmission electron microscopy (TEM) revealed rod-like ChNCs (543.71 nm length, 48.70 nm width) and web-like ChNFs (61.15 nm width). Fouriertransform infrared spectroscopy (FTIR) confirmed successful surface carboxylation, with degrees of substitution of 0.32 for ChNCs and 0.28 for ChNFs. Both nanomaterials exhibited high crystallinity (91.55% for ChNCs, 87.65% for ChNFs), negative zeta potential values (−44.56 mV for ChNCs, −16.93 mV for ChNFs), and enhanced thermal stability compared to raw chitin. The process, evaluated using sustainability metrics, yielded an E-factor of 3.317, highlighting significant waste reduction over conventional acid hydrolysis. This eco-friendly approach aligns with green chemistry principles and offers a sustainable, scalable solution for chitin nanomaterial production, suitable for diverse industrial applications.