Developing banking services based on technology is an inevitable and objective trend in the era of international economic integration. This study aims to determine the factors impacting the adoption and use of online banking services in Vietnam. The proposed research model is based on the adjustment of Unified Theory of Acceptance and Use of Technology (UTAUT2). We employed the structural equation modeling (SEM) and artificial neural network model (ANN) to comprehensively evaluate the linear and non-linear effects of factors on the adoption and use of online banking services in Vietnam. With survey data of 433 customers from three key economic areas in Vietnam, the result shows that the factors of expected efficiency, cost, expected effort, brand image, perceived risk, and social influence impact behavioral intention to use online banking services. At the same time, the behavioral intention to use online banking services also increases the decision to choose online banking services. Based on the results, we propose some implications for Vietnamese commercial banks to increase the acceptance of online banking.