Water quality is under constant threat worldwide due to the discharge of heavy metals into the water from industrial waste. In this report, we introduce a potential candidate, chitosan, extracted and isolated from shrimp shells, that can adsorb heavy metals from polluted water. The waste shrimp shell chitosan was characterized via Fourier transform infrared spectroscopy (FTIR) and scanning electron microscopy with energy dispersive X-ray spectroscopy (SEM-EDS). The adsorption capacity of heavy metals on the modified shrimp shell was measured using an inductively coupled plasma mass spectrometry before and after adsorption. The highest adsorption of arsenic, nickel, and cobalt was 98.50, 74.50, and 47.82%, respectively, at neutral pH, whereas the highest adsorption of chromium was 97.40% at pH 3. Correspondingly, the maximum adsorption capacities of MSS for As, Cr, Ni, and Co were observed to be 15.92, 20.37, 7.00, and 6.27 mg/g, respectively. The application of Langmuir and Freundlich isotherm models revealed that the adsorption processes for the heavy metals were statistically significant (r2 > 0.98). The kinetic studies of metal adsorption, using modified shrimp shell, were well explained by the pseudo-second-order kinetic model with linear coefficients (r2) of >0.97. The presence of a greater number of functional groups on the adsorbent, such as N–H coupled with H–O, –COO−, C–H, N–N, and C–O–C, was confirmed by FTIR analyses. Furthermore, SEM-EDX analysis detected the presence of elements on the surface of modified shrimp shell chitosan. This noteworthy adsorption capacity suggests that MSS could serve as a promising, eco-friendly, and low-cost adsorbent for removing toxic heavy metals including Cr, Ni, As, and Co and can be used in many broad-scale applications to clean wastewater.