The lunar nearside large volcanic complexes, such as the Rümker Hills, Aristarchus Plateau, and Marius Hills are likely sites of intense and sustained magmatic activity. These volcanic complexes, recently proposed to be shield volcanoes, are generally located at regionally high elevations and some feature relatively well-localized positive gravity anomalies. Applying localized spectral analyses on high-resolution gravity data obtained from the Gravity Recovery and Interior Laboratory (GRAIL) mission and topography data returned from the Lunar Reconnaissance Orbiter (LRO) spacecraft, we study the subsurface structures of these volcanic complexes. The gravity signal is predicted using a thin elastic lithospheric model that considers both surface and subsurface loads. Best-fit crustal and load densities show that the topographic highs of Rümker Hills, Marius Hills, Gardner and Kepler are mainly composed of material that has a density of more than 2850kgm−3, which is consistent with that of emplaced igneous rocks. Both the Aristarchus Plateau and Hortensius have relatively lower crustal and surface load densities, with mean values around 2550kgm−3, which are well consistent with the average bulk density of the lunar highland crust. These results, together with evidence of multiple volcanic edifices on the surface, suggest that the shallow crusts of the Rümker Hills, Marius Hills, Gardner and Kepler are mainly composed of dense intrusive/extrusive magmatic units, and those of the Aristarchus Plateau and Hortensius are mainly composed of low density materials with only small amounts of superimposed volcanic material. To further constrain the subsurface structures beneath these volcanic complexes, we analyze the Bouguer gravity anomalies for these regions. Results show that dense materials that might be solidified intrusions exist beneath Rümker Hills, Marius Hills, Gardner and Prinz, but no substantial dense materials have been detected beneath the Aristarchus Plateau, Hortensius, Kepler or Cauchy. The different subsurface structures among these large volcanic complexes suggest that the volcanism style at the lunar nearside is different from each other, even for those formed at the same geological time.