<p>Earlier research highlighted that smartphone has been used at work for private activities and at home for work-related tasks with differing outcomes. Because smartphone use to simultaneously conduct professional and private activities at home differs from previous studies, different outcomes can be expected. The current study, therefore, examined the underexplored smartphone use to simultaneously conduct private and work-related tasks at home as underlying mechanism of the relationship between work pressure and work-life balance (WLB). The study equally explored whether self-regulation moderates the mediation effect of smartphone use on WLB among 519 university academics sampled from federal universities in South-eastern Nigeria. Results of Hayes’ PROCESS Model 14 indicated that work pressure significantly related to WLB only through smartphone concurrently used to conduct private and work-related tasks at home. Self-regulation significantly moderated the mediation effect of smartphone use such that the indirect effect of work pressure on WLB through smartphone use is more pronounced at lower levels of self-regulation and diminishes as self-regulation increases. Our findings deepen the understanding of how work pressure impairs WLB through smartphone use to conduct work-related and private activities at home, but illuminate how employees can deal with work pressure to attain WLB. </p>