A nanopillar assisted multilayer antireflection (AR) coating that combines the Ta2O5/SiO2 multilayer with SiO2 nanopillars was investigated to improve the light absorption of quadruple-bandgap photovoltaics. After clarifying that the performance of the traditional multilayer AR coating is restricted by the available refractive index of the top layer, periodic SiO2 rhombic nanopillars that work in the subwavelength regime were used to vary its effective index from 1 to 1.46. Then, the effective index and thickness of SiO2 nanopillars were optimized together with the Ta2O5/SiO2 stack using the global optimization algorithm to further reduce the reflection loss. When the SiO2 nanopillars have an effective index of 1.15 and a thickness of 108 nm, the best AR performance was achieved with a reflectance of 3.9% in the target spectral range of 300–1700 nm. Using laser interference lithography and ion assisted deposition technologies, the nanopillar assisted AR coating was realized with a reflectance of 4.5%. Compared to the traditional multilayer AR coating, this hybrid approach can not only achieve better AR performance but also reduce the disparities of the reflection loss among different bandgaps, which helps us to effectively improve the current matching and enhance the overall efficiency of quadruple-bandgap photovoltaics.