Examining the reflectance of the Moon’s surface across a broad range of viewing geometries through photometric analysis can reveal physical and geological properties of its regolith. Since 2013 December, the Lunar Orbiter Laser Altimeter (LOLA) on board the Lunar Reconnaissance Orbiter (LRO) has been operating as a near-infrared (1064 nm) passive radiometer when its laser is turned off. We present a new analysis of this data set spanning roughly 8 yr and covering the surface up to high latitudes in both hemispheres. We apply semiempirical phase functions to find a lower photometric slope and a narrower opposition effect for the highlands than the maria, consistent with theoretical expectations given the higher albedo of the highlands. Examining various geological properties at global scales shows that, in the highlands, iron abundance (FeO) and optical maturity (OMAT) are the dominant factors affecting the phase function, with a smaller influence from surface slope. In the maria, FeO is the dominant factor, with smaller influences from OMAT, surface slope, and TiO2. Submicroscopic iron abundance (SMFe) has a similar effect to OMAT in both highlands and maria. Analysis at specific sites, including the Reiner Gamma swirl and several silicic anomalies, indicates that the phase functions are consistent with the global data for similar FeO and OMAT. Thermophysical properties inferred from surface temperature observations by the Diviner Lunar Radiometer Experiment on board LRO do not affect the 1064 nm phase function, possibly due to a difference between their depth scale and LOLA’s sensing depth.