Arsenic is a deleterious heavy metal that is usually removed from polluted water based on adsorption processes. The latest mode of modeling such a process is to implement artificial intelligence (AI). In the current work, a new artificial neural network (ANN) model was developed to predict the adsorption efficiency of arsenate (As(III)) from contaminated water by analyzing different architectures of an adaptive network-based fuzzy inference system (ANFIS). The database for the current study consisted of the experimental data of the adsorption of As(III) by different adsorbents/biosorbents. The data were randomly divided into two sets: 70% for the training phase and 30% for the testing phase. Four statistical evaluation metrics, namely, mean square error (MSE), root-mean-square error (RMSE), Pearson’s correlation coefficient (R%), and the determination coefficient (R2) were used for the analysis. The best performing ANFIS model was characterized with the average values of 97.72%, 0.9333, 0.137, and 0.274 of R%, R2, MSE, and RMSE, respectively. In addition, a parametric investigation revealed that the most dominating parameters on the adsorption process efficiency were in the following order: pH, As initial concentration, contact time, adsorbent dosage, inoculum size, and temperature. The results of the current study would be useful in the adsorption process scale-up and optimization.