Highlighted by the discovery of high-temperature superconductivity, strongly correlated oxides with highly distorted perovskite structures serve as intriguing model systems for pursuing emerging materials physics and testing technological concepts. While 3d correlated oxides with a distorted perovskite structure are not uncommon, their 4d counterparts are unfortunately rare. In this work, we report the tuning of the electrical and optical properties of a quasi-2D perovskite niobate CsBiNb2O7 via hydrogenation. It is observed that hydrogenation induces drastic changes of lattice dynamics, optical transmission, and conductance. It is suggested that changing the orbital occupancy of Nb d orbitals could trigger the on-site Coulomb interaction in the NbO6 octahedron. The observed hydrogen doping-induced electrical plasticity is implemented for simulating neural synaptic activity. Our finding sheds light on the role of hydrogen in 4d transition metal oxides and suggests a new avenue for the design and development of novel electronic phases.