Within this work was explored the influence of nickel oxide decoration on the photoconductive effects exhibited by multiwall carbon nanotubes. Samples in thin film form were prepared by a chemical vapor deposition method. Experiments for evaluating the photo-response of the nanomaterials at 532 nanometers wavelength were undertaken. A contrasting behavior in the photoelectrical characteristics of the decorated nanostructures was analyzed. The decoration technique allowed us to control a decrease in photoconduction of the sample from approximately 100μmhos/cm to −600μmhos/cm. Two-wave mixing experiments confirmed an enhancement in nanosecond nonlinearities derived by nickel oxide contributions. It was considered that metallic nanoparticles present a strong responsibility for the evolution of the optoelectronic phenomena in metal/carbon nanohybrids. Impedance spectroscopy explorations indicated that a capacitive behavior correspond to the samples. A potential development of high-sensitive Wheatstone bridge sensors based on the optoelectrical performance of the studied samples was proposed.