Research on the use of smartphone apps with the aim of developing self-regulated learning (SRL) and increasing academic performance of university students in virtual mode, as a result of the COVID-19 pandemic, is recent and scarce. The present article shows the results of a study that analyzed the effect of using the 4Planning app with an intra-curricular approach on SRL and on the academic performance of 119 1st-year psychology students in virtual mode, at a Chilean university (MAge = 22.81, SDAge = 6.52). The research was conducted with quantitative methodology and a quasi-experimental design, with pre- and posttest measurements of an experimental group and comparisons with three control groups. The results show that students who used the app during 10 weeks of the first academic semester 2021: (1) increased SRL self-report, (2) increased academic self-efficacy, and (3) obtained higher academic performance, compared to those who did not use it. The above occurs because the 4Planning app activates functions of the self-regulatory system of goal-directed behavior, which allows exercising the capacity of self-direction and self-influence on this type of behavior in the particular context of academic performance, which produces SRL. It is concluded that the 4Planning app is effective in developing self-regulation and improving the academic performance of 1st-year university students, in virtual learning mode.