Contradictory results in the extant literature suggests that additional risk factors should be considered when exploring the impacts of maternal smartphone use on mother‐infant relationships. This study used cluster analysis to explore whether certain risk factors were implicated in mother‐infant dyads with high smartphone use and low mother‐infant responsiveness. A cross‐sectional survey of 450 participants in the UK measured infant social‐emotional development, maternal depressive, anxiety and stress symptoms, wellbeing, social support, smartphone use, and mother‐infant responsiveness. Participants were predominantly White (95.3%) and living with a partner (95.2%), with infants who were born full‐term (88.9%). Cluster analysis identified three clusters characterized as; cluster (1) “infant at risk” showing high infant development concerns, high maternal smartphone use, and low mother‐infant responsiveness; cluster (2) “mother at risk” showing high maternal depressive, anxiety, and stress scores, low social support, high maternal smartphone use, and low mother‐infant responsiveness, and cluster (3) “low risk” showing low maternal smartphone use and high mother‐infant responsiveness. Significant differences were found between all risk factors, except for maternal smartphone use and mother‐infant responsiveness between clusters 1 and 2 suggesting that both clusters require early intervention, although interventions should be tailored towards the different risk factors they are presenting with.