An ordered macroporous Beta zeolite (OMbeta) support was synthesized via a bottom-up templating strategy and used to prepare a highly active Ni2P (nickel phosphide) catalyst for hydrodenitrogenation (HDN). The formation mechanism of the ordered porous Beta zeolite was elucidated through detailed characterization. SEM images reveal that the Beta zeolite is composed of ∼250 nm spherical crystals, densely packed in an opal-like arrangement, with ∼55 nm voids forming between the crystallites due to shrinkage during synthesis. This interconnected microporous–macroporous structure significantly improves reactant diffusion and facilitates uniform Ni2P dispersion. As a result, the Ni2P/OMbeta catalyst exhibits enhanced quinoline HDN activity compared to Ni2P supported on conventional Beta zeolite.