This paper is devoted to the development and construction of a practical Machine Learning (ML)-based model for the prediction of tensile strength of polymer carbon nanotube (CNTs) composites. To this end, a database was compiled from the available literature, composed of 11 input variables. The input variables for predicting tensile strength of nanocomposites were selected for the following main reasons: (i) type of polymer matrix, (ii) mechanical properties of polymer matrix, (iii) physical characteristics of CNTs, (iv) mechanical properties of CNTs and (v) incorporation parameters such as CNT weight fraction, CNT surface modification method and processing method. As the problem of prediction is highly dimensional (with 11 dimensions), the Gaussian Process Regression (GPR) model was selected and optimized by means of a parametric study. The correlation coefficient (R), Willmott’s index of agreement (IA), slope of regression, Mean Absolute Percentage Error (MAPE), Root Mean Squared Error (RMSE) and Mean Absolute Error (MAE) were employed as error measurement criteria when training the GPR model. The GPR model exhibited good performance for both training and testing parts (RMSE = 5.982 and 5.327 MPa, MAE = 3.447 and 3.539 MPa, respectively). In addition, uncertainty analysis was also applied to estimate the prediction confidence intervals. Finally, the prediction capability of the GPR model with different ranges of values of input variables was investigated and discussed. For practical application, a Graphical User Interface (GUI) was developed in Matlab for predicting the tensile strength of nanocomposites.