In this study, we utilized lime mud waste from paper mills to synthesize calcium hydroxide (Ca(OH)2) nanoparticles (NPs) and investigate their application for the removal of phosphorus from aqueous solution. The NPs, composed of green portlandite with hexagonal shape, were successfully produced using a precipitation method at moderately high temperature. The crystal structure and characterization of the prepared Ca(OH)2 nanoparticles were analyzed by field emission scanning electron microscopy, Fourier transform infrared spectroscopy, and X-ray diffraction. The effects of Ca(OH)2 NP dosage and contact time on removal of phosphorus were also investigated. The results show that the green portlandite NPs can effectively remove phosphorus from aqueous solution. The phosphorus removal efficiencies within 10 min are 53%, 72%, 78%, 98%, and 100% with the different mass ratios of Ca(OH)2 NPs/phosphorus (CNPs/P) of 2.2, 3.5, 4.4, 5.3, and 6.2, respectively. Due to the efficient phosphorus removal, the calcium hydroxide nanoparticles (CNPs) could be a potential candidate for this application in domestic or industrial wastewater treatment.