A full-duplex radiant energy converter based on both betavoltaic and photovoltaic effects in an easy-to-implement way is an attractive alternative for the autonomous wireless sensor microsystem. Here, we report a novel beta/photovoltaic cell based on free-standing ZnO nanorod arrays (ZNRAs) modified with metallic single-walled carbon nanotubes (m-SWCNTs), using radioisotope 63Ni as beta-emitting source. The ZNRAs were grown on Al-doped ZnO (AZO) conductive glass using hydrothermal method. The optimum length and diameter of ZnO nanorods were determined by Monte Carlo simulation for beta energy deposition in ZNRAs. The m-SWCNTs were anchored into the ZNRAs to form a three-dimensional (3-D) Schottky junction structure for effectively separating the beta/photo-excited electron-hole pairs. Experimentally, the betavoltaic and photovoltaic effects were confirmed through the I–V measurements of beta/photovoltaic cells under beta/UV/Vis irradiations, respectively. It is suggested that the m-SWCNTs play key role for the enhancement of beta/photovoltaic performance through the formation of extensive 3-D Schottky junction, the conductive network for hole transport, and the surface plasmon resonance exciton absorption for visible light.