This study synthesized NiAl-layered double hydroxide (LDH)/Cu-MOF photocatalyst using a simple impregnation method involving NiAl-LDH and Cu-MOF. The successful synthesis was confirmed through Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), scanning electron microscopy (SEM), zeta potential measurements, thermogravimetric analysis (TGA), ultraviolet diffuse reflectance spectroscopy (UV-DRS), N2 adsorption at −196 °C, and electrochemical impedance spectroscopy (EIS). Photocatalysts based on NiAl-LDH, Cu-MOF, and NiAl-LDH/Cu-MOF were used to remove methyl orange (MO) dye from contaminated water. The impact of various factors, including pH, dye concentration, and photocatalyst amount, on MO degradation efficiency was assessed. FTIR analysis was conducted both before and after dye degradation. The optimal degradation conditions were a photocatalyst dose of 25 mg and a pH of 3. Kinetic studies indicated that the degradation of MO dye onto NiAl-LDH/Cu-MOF followed a pseudo-first-order and an L–H or Langmuir–Hinshelwood model. The value of R2 = 0.94 confirms the validity of pseudo-first-order and Langmuir–Hinshelwood (L–H) kinetic models for the photocatalytic degradation of MO dye. This study highlights the importance of developing novel photocatalysts with improved degradation efficiency to protect the water environment. Antibacterial activity was also performed with antibacterial sensibility testing by disk diffusion to determine minimal inhibitory and bactericidal concentrations. In short, NiAl-LDH/Cu-MOF can be helpful for various biomedical and industrial applications.