This study introduces a novel chitosan-immobilised imino-phosphorane composite (Chi-iph) for the efficient removal of lead (Pb2+) and chromium (Cr3+) from wastewater. The successful synthesis of Chi-iph was confirmed using FT-IR, XPS, BET, EDX, TGA, 1H-NMR, 13C-NMR, EI/MS, and ICP-OES analyses. Various experimental parameters such as pH, equilibrium time, metal concentration, adsorbent dose, temperature, and eluents were optimised to enhance the adsorption performance. At 25°C, with pH values of 5.5 for Pb2+ and 4.5 for Cr3+, an initial concentration of 200 mg/L, and an agitation time of 20 min, the maximum adsorption capacities were 55 mg/g for Pb2+ and 45 mg/g for Cr3+. Kinetic modelling demonstrated that the pseudo-first-order model best predicted the adsorption process, yielding capacities of 56.65 mg/g for Pb2+ and 46.38 mg/g for Cr3+. Isotherm analysis showed that the Langmuir model was a better fit than the Freundlich model, with theoretical capacities of 56.81 mg/g for Pb2+ and 44.64 mg/g for Cr3+. The Dubinin–Radushkevich (D-R) isotherm revealed adsorption energy (E) values of 9.45 kJ/mol for Pb2+ and 8.64 kJ/mol for Cr3+, indicating a chemisorption process. Theoretical saturation capacities (qD) were 56.28 mg/g for Pb2+ and 45.58 mg/g for Cr3+. Temkin isotherm results, with bT values of 9.71 and 8.53 kJ/mol for Pb2+ and Cr3+ respectively, aligned closely with the D-R model, further confirming chemisorption. Thermodynamic studies indicated that the adsorption process is exothermic, spontaneous, and more favourable at lower temperatures. Complete desorption of the heavy metals was achieved using 1 M HNO₃, allowing for efficient metal recovery. In a practical application, the Chi-iph composite removed 11.5 mg/L of Pb2+ and 7.01 mg/L of Cr3+ from contaminated wastewater, demonstrating its potential for environmental remediation. The composite’s performance aligns with WHO and FAO guidelines, making it suitable for treating wastewater before disposal into marine environments.