Herein, a simple and portable electrochemical sensor based on a reduced graphene oxide/gold nanoparticle/manganese dioxide (rGO/AuNP/MnO2) nanocomposite-modified screen-printed carbon electrode (SPCE) was constructed by the facile stepwise electrodeposition method and used for electrochemical detection of As(III). The resultant electrode was characterized for its morphological, structural, and electrochemical properties using scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), energy dispersive X-ray spectroscopy (EDX), cyclic voltammetry (CV), and electrochemical impedance spectroscopy (EIS). From the morphologic structure, it can be clearly observed that the AuNPs and MnO2alone or their hybrid were densely deposited or entrapped in thin rGO sheets on the porous carbon surface, which may favor the electro-adsorption of As(III) on the modified SPCE. It is interesting that the nanohybrid modification endows the electrode with a significant decrease in charge transfer resistance and an increase in electroactive specific surface area, which dramatically increases the electro-oxidation current of As(III). This improved sensing ability was ascribed to the synergistic effect of gold nanoparticles with excellent electrocatalytic property and reduced graphene oxide with good electrical conductivity, as well as the involvement of manganese dioxide with a strong adsorption property in the electrochemical reduction of As(III). Under optimized conditions, the sensor can detect As(III) via square wave anodic stripping voltammetry (SWASV) with a low limit of detection of 2.4 μg L−1and a linear range of 25–200 μg L−1. The proposed portable sensor shows the advantages of a simple preparation procedure, low cost, good repeatability, and long-term stability. The feasibility of rGO/AuNPs/MnO2/SPCE for detecting As(III) in real water was further verified.