Optimization of bifunctional Ni catalysts was performed to enhance the catalytic performance in the one-pot synthesis of commercially valuable menthol from citral. The effect of nickel precursors (nitrate, chloride, acetate, and sulfate) and the addition of bentonite clay was investigated in citral transformations in a batch reactor at 70 °C and 10 bar hydrogen, demonstrating higher activity for the Ni-H-β-38-bentonite composite derived from a nickel nitrate precursor, which can be attributed to a higher surface area, optimal Brønsted to Lewis acidity and metal particle size, as well as the egg-shell distribution of Ni particles. H-β-38 impregnated with nickel nitrate, followed by calcination and reduction, was shaped with bentonite as a binder to give extrudates for exploring the citral transformations in the trickle-bed reactor at 50–70 °C and 10 bar hydrogen. The highest selectivity to the desired menthols of 45% was obtained with 70% stereoselectivity to the menthol isomer at 70 °C. The apparent activation energy for citral transformations to menthols of 18.6 kJ/mol indicated the presence of mass transfer limitations. Catalytic activity was linked with the physical-chemical properties, which were characterized by transmission electron microscopy, X-ray diffraction, temperature-programmed reduction, Fourier transform infrared spectroscopy with pyridine, N₂ physisorption, and inductively coupled plasma–optical emission spectrometry methods.