This paper presents a new hybrid approach for the prediction of functional properties i.e., self-cleaning efficiency, antimicrobial efficiency and ultraviolet protection factor (UPF), of titanium dioxide nanoparticles (TiO2 NPs) coated cotton fabric. The proposed approach is based on feedforward artificial neural network (ANN) model called a multilayer perceptron (MLP), trained by an optimized algorithm known as crow search algorithm (CSA). ANN is an effective and widely used approach for the prediction of extremely complex problems. Various studies have been proposed to improve the weight training of ANN using metaheuristic algorithms. CSA is a latest and an effective metaheuristic method relies on the intelligent behavior of crows. CSA has been never proposed to improve the weight training of ANN. Therefore, CSA is adopted to optimize the initial weights and thresholds of the ANN model, in order to improve the training accuracy and prediction performance of functional properties of TiO2 NPs coated cotton composites. Furthermore, our proposed algorithm i.e., multilayer perceptron with crow search algorithm (MLP-CSA) was applied to map out the complex input-output conditions to predict the optimal results. The amount of chemicals and reaction time were selected as input variables and the amount of titanium dioxide coated on cotton, self-cleaning efficiency, antimicrobial efficiency and UPF were evaluated as output results. A sensitivity analysis was carried out to assess the performance of CSA in prediction process. MLP-CSA provided excellent result that were statistically significant and highly accurate as compared to standard MLP model and other metaheuristic algorithms used in the training of ANN reported in the literature.