Biguanidine-functionalized chitosan was synthesized and combined with Pd NPs to yield a recyclable, environment-friendly heterogeneous catalytic system for the Suzuki-Miyaura C-C coupling reaction. The catalysts were characterized with FTIR, TEM, SEM, EDX, WDX, ICP, and XPS. The catalyst is used in Suzuki cross-coupling reaction of various aryl halides, including less reactive chlorobenzene, and phenylboronic acid to give biaryls without any additive or ligand. A reusability test demonstrated that the catalysts were highly efficient even after six run. The solid-phase poisoning and leaching tests indicated that the catalysts have heterogeneous nature.