In this study, we aimed to synthesize and characterize a nickel(II) complex-modified graphene oxide (Ni-GO) nanocomposite with enhanced photocatalytic and antimicrobial properties. The nanocomposite was prepared through a modified Hummer’s method, followed by an adsorption technique using the precursor complex [Ni(bipy)3]Cl2·5H2O, which was preferentially adsorbed onto the graphene oxide (GO) surface. The surface interaction between the nickel complex ions and GO was characterized using various analytical techniques, including FTIR, XRD, SEM-EDX, DRS, and XPS analyses. Photoluminescence analysis demonstrated the fluorescence property of the prepared composite. The DRS spectra indicated that the adsorption of composite particles extended to the visible region, making it excitable by visible light. The photocatalytic activity of the Ni-GO nanocomposite was tested by studying the degradation of an organic model pollutant, Rhodamine B dye, under real sunlight irradiation. The introduction of the Ni(II) complex onto the GO surface matrix intensified the photocatalytic property, making it more efficient under direct sunlight exposure. Comparisons with pristine graphite and GO revealed that Ni-GO exhibited enhanced photocatalytic potential. Additionally, we have evaluated the antimicrobial property of the Ni(II) complex-modified GO against Klebsiella pneumoniae. The results demonstrated that both the Ni(II) precursor complex and Ni-GO nanocomposite possessed an excellent antimicrobial efficacy, suggesting their potential use in antimicrobial applications. The synthesis and characterization of the Ni(II) complex-modified GO nanocomposite presented in this study showed promising results for both ameliorative photocatalytic and antimicrobial activities. These findings indicated the potential utility of Ni-GO as an efficient photocatalyst and antimicrobial agent, surpassing the performance of pristine graphite and GO. This research opens up new avenues for the development of advanced nanocomposites with diverse applications in environmental remediation and biomedical fields.