The main threats from heavy metals specifically arsenic-contaminated drinking water have been emerging as an environmental and social crucial issue. Herein, the arsenic (V) (As(V)) biosorption performance of waste orange peel (OP) driven-graphene-like porous carbon (GPC) was investigated experimentally and an artificial neural network (ANN) approach was used to model the biosorption process. The initial pH (2.0, 3.0, 4.0, 5.0, 6.0, 7.0, 8.0, and 10.0), initial As(V) concentration (25.0, 50.0, 100.0, 250.0, 500.0 and 750.0 mg.L -1 ), biosorbent dosage (1.0, 2.0, 3.0, 4.0 and 5.0 g.L -1 ), and contact time (0-120.0 min) were investigated to optimize the biosorption process. The as-synthesized GPC biosorbents with a high specific surface area (985 m 2 .g -1 ) and pore volume (1.04 cm 3 .g -1 ) offered superior removal efficiency as 88.2% (equilibrium uptake capacity of 46.5 mg.g -1 ) at initial pH 6.0, initial As(V) concentration 100 mg.L -1 , and biosorbent dosage 2.0 g.L -1 . A three-layer ANN model was developed to forecast the Ar(V) biosorption performance of GPCs. Several experimental data points were considered as test data to validate the ANN model. The ANN model was performed with the Levengberg-Marquardt algorithm (LMA), linear transfer function (purelin) at the output layer, and a tangent sigmoid transfer function (tansig) in the hidden layer with 12 neurons. The values of coefficient of determination and mean squared error were calculated to be 0.9858 and 0.0014, respectively. The results revealed that the experimental data were in accordance with ANN-driven data as well as reveling the high accuracy of the ANN approach in estimating the target variable. The developed ANN model is useful for the optimization of process conditions for pilot-scale utilization of As(V) biosorption process by GPC.