Background Augmented reality (AR) is a novel modality for promoting smoking cessation (SC). AR-visualized adverse consequences for education and smoking prevention have only been evaluated in nonsmokers in previous studies. Objective To assess the feasibility and preliminary effectiveness for SC of AR pictorial health warnings (PHWs) on cigarette packs. Methods We conducted a pilot randomized controlled trial in adult daily smokers in communities in Hong Kong. All participants received AWARD (ask, warn, advise, referral, do-it-again) model–guided SC advice, a warning leaflet, and referral to SC services at baseline. Interactive, chat-based SC support comprising regular messages and real-time support was provided to all participants via instant messaging apps (eg, WhatsApp) for 3 months after randomization. Participants in the intervention group additionally received 6 links to the AR PHWs showing the worsening health status of various organs caused by smoking. The level of the AR PHWs was adjustable to smoking behaviors (ie, smoking duration or daily cigarette consumption) to increase interaction. Participants could swipe, drag, or rotate the 3D PHWs to reinforce their impression of the health consequences of smoking. The primary outcome was self-reported past 7-day point-prevalence abstinence (PPA) at 3 months. The acceptability of the AR intervention was assessed by the proportion of participants who had viewed AR PHWs during the intervention. Participants who viewed AR PHWs further evaluated the perceived effect of the AR PHWs on a scale of 0 (not helpful at all) to 10 (very helpful). Intention to treat was used, and the risk ratio (RR) of the intervention effect was estimated by Poisson regression. Results From April to November 2021, 80 participants were recruited and randomly assigned to intervention (n=40) and control (n=40) groups. Most participants were male (66/80, 83%) and planned to quit beyond 30 days or were undecided (65/80, 81%). The intervention group had a higher but nonsignificant 7-day PPA (7/40, 18% vs 5/40, 13%; RR 1.40, 95% CI 0.48-4.07) and quit attempts (15/40, 38% vs 11/40, 28%; RR 1.36, 95% CI 0.71-2.60) at 3 months than the control group. In the intervention group, 17 of 40 (43%) participants viewed the AR PHWs. The AR PHWs had modest effects on knowledge of the adverse consequences of smoking on personal health (mean score 3.94, SD 3.52), reducing the frequency of buying cigarettes (mean score 3.29, SD 3.08), increasing the perceived importance of quitting (mean score 3.88, SD 3.50), and making the PHWs more disgusting (mean score 3.41, SD 3.08) and horrible (mean score 3.38, SD 3.05). The 3-month self-reported 7-day PPA was higher in those who ever (vs never) viewed the AR PHWs (5/17, 29% vs 2/23, 9%). Conclusions The mobile-based interactive AR PHWs were feasible, and the effectiveness on smoking abstinence warrants further testing. Trial Registration ClinicalTrials.gov NCT04830072; https://clinicaltrials.gov/study/NCT04830072