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The crystal structure, morphology, and linear and nonlinear optical properties of Co-doped Ba1−xCoxTiO3 (x = 0.00, 0.02, 0.03, 0.04, and 0.06) were investigated using x-ray diffraction (XRD), scanning electron microscopy, and UV–visible spectroscopy measurements. The XRD patterns confirmed that the Ba1−xCoxTiO3 samples crystallized in the perovskite phase, and a transition from quadratic to pseudo-cubic phase was observed with Co doping. Upon doping, the band gap (Eg) decreased from 3.14 eV to 2.11 eV, indicating that Co doping into BaTiO3 caused a change in their electronic levels associated with lattice defects. Additionally, the optical parameters including linear refractive index, extinction coefficient, dielectric coefficient, optical conductivity (σopt), and the static index (n0) were extracted and linked to the Co content. Finally, analysis of the linear (LOp) and nonlinear optical (NLOp) parameters of Ba1−xCoxTiO3 revealed that the increase in Co content induces an increase in the NLOp refractive index (n2) and third-order NLOp susceptibility χ(3). [ABSTRACT FROM AUTHOR]