A microwave-assisted synthesis of a NiTiO3-based chitosan (NT/CS) nanocomposite with acceptable pseudocapacitive performance is reported. The requisite NiTiO3 nanoparticles were prepared by a simple, ultrafast, one-pot combustion technique activated by microwave heating at a power of 900 W for 20 min. This combustion reaction was performed in the solid state, using urea and ammonium nitrate as fuel and oxidant, in a home-made set-up encircled by a CuO jacket to capture microwave radiation. Detailed study of the structural and morphological characteristics of the resulting products revealed successful fabrication of NiTiO3 and NiTiO3/CS particles with pure phases and average particle sizes of about 30 and 39 nm, respectively. The pseudocapacitive behavior was evaluated through a series of electrochemical tests, including cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) at different scan rates and potentials. The results indicated an increased specific capacitance (197 F g−1) for the prepared NT/CS film compared to that of pristine chitosan (76 F g−1) at a potential scan rate of 10 mV s−1. Further CV examination after 2000 cycles revealed a capacity retention of around 86%, indicating good recyclability and a long cycle life. The band-gap energy of the product and its relationship with specific capacitance is also discussed in detail. The obtained results show the product to be highly promising as an electrode material in electrochemical applications.