Research Highlights: This study examined the emotional and cognitive health benefits of nature in comparison with working memory training. It considered the long-term effects, the application of mobile terminal technology, and routine-based approaches with the aim of integrating nature’s health benefits into people’s daily lives. Background and Objectives: Infectious diseases and aging may limit people’s activities indoors; the recovery effect of nature has been widely recognized, and terminal technology is developing rapidly. In this context, we want to explore the emotional and cognitive effects of viewing nature (VR) videos on mobile devices for a long time. Materials and Methods: The experiment employed a between-subjects design, with participants being randomly assigned to one of four groups: a forest VR video group, a water VR group, a working memory training group, and a control group. The participants watched the video three times a week for 20 min each for four weeks. The number of valid participants for compliance, preference, and willingness was 136, and the number of valid participants for the study of emotional and cognitive effects was 62. Brief Profile of Mood States (BPOMS) scales, running memory accuracy, shifting cost, etc., were used as indicators to reflect emotions and cognition. A repeated measures analysis of variance was performed on these indicators at four groups × two time points (pretest/post-test). Results: ① There were no significant differences in the participants’ adherence, preferences, and willingness to watch different natural videos and perform working memory training. ② Long-term home training (e.g., watching VR nature videos or working memory training) may have had a minimal effect on emotional responses to mobile terminals. However, home training may be more conducive to the stabilization of anger. ③ Watching forest VR videos had a positive effect on the updating function of the brain; watching water VR videos was beneficial for the shifting function and automatic processing speed; and working memory training had a positive effect on the updating and shifting functions. Conclusions: There were no significant differences in adherence, preference, willingness, and effects on emotion and cognition between long-term forest VR video viewing, water VR video viewing, and working memory training on mobile terminals. All three types of home training may be beneficial for the stabilization of emotion (especially anger), and all can have some positive effects on cognition.