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Background The COVID-19 pandemic has been highly disruptive, with the closure of schools causing sudden shifts for students, educators and parents/caregivers to remote learning from home (home-schooling). Limited research has focused on home-schooling during the COVID-19 pandemic, with most research to date being descriptive in nature. The aim of the current study was to comprehensively quantify the psychosocial impacts of home-schooling on parents and other caregivers, and identify factors associated with better outcomes. Methods A nationally representative sample of 1,296 Australian adults was recruited at the beginning of Australian COVID-19 restrictions in late-March 2020, and followed up every two weeks. Data for the current study were drawn from waves two and three. Surveys assessed psychosocial outcomes of psychological distress, work and social impairment, and wellbeing, as well as a range of home-schooling factors. Results Parents and caregivers who were home-schooling during the COVID-19 pandemic experienced significantly higher levels of psychological distress and work/social impairment compared to those who were not home-schooling or had no school-aged children. A current mental health diagnosis or lower levels of perceived support from their child’s school negatively affected levels of psychological distress, work and social impairment, and wellbeing in parents and caregivers involved in home-schooling. Conclusions The mental health impacts of home-schooling were high and may rise as periods of home-schooling increase in frequency and duration. Recognising and acknowledging the challenges of home-schooling is important, and should be included in psychosocial assessments of wellbeing during periods of school closure. Emotional and instrumental support is needed for those involved in home-schooling, as perceived levels of support is associated with improved outcomes. Proactive planning by schools to support parents may promote better outcomes and improved home-schooling experiences for students.