Introduction There are many orphaned and separated children (OSC) in the world and caregivers play a crucial role in raising them. Frameworks on employee mental health incorporate elements of both enjoyment/difficulties and values (i.e., hedonic and eudaimonic elements), yet existing studies focus on caregivers’ mental illness and overlook their specific work activities. Methods We collected diary activity log, survey, and interview data from caregivers from five geographic locations: Hyderabad, India; Nagaland, India; Ethiopia; Kenya; and Cambodia. We coded and calculated the amount of time spent on five frequent activities: cleaning, cooking, caring for children, supervising children, and informal educational activities. We calculated the mean scores of perceived importance, meaningfulness, enjoyment, and unpleasantness for each of the five activities by geographic location. Results A total of 82 participants completed surveys and activity logs, and 69 of them participated in interviews. Mean time spent per day for the five activities combined ranged from 4.4 h (Nagaland) to 9.0 h (Ethiopia). Cooking and cleaning constituted a large portion of caregivers’ days, ranging from 0.8 h per caregiver per day in Nagaland to 4.7 h in Cambodia, and informal educational activities (such as advising, teaching children their letters, and teaching from religious texts) constituted the least time, ranging from 0.1 h per caregiver per day in Hyderabad to 1.1 h in Nagaland. Participants rated all activities high in importance, with cleaning being relatively lower. Overall, enjoyment scores were lower than importance and meaningfulness scores. Informal educational activities had the highest enjoyment scores in three locations, whereas supervising children did in two locations. Participants rated cleaning as the most unpleasant activity in each geographic region except Cambodia, where it was rated on par with educational activities. Discussion OSC caregivers consider several regular activities to be very important and meaningful. Enjoyment may be improved through additional support in child behavior management or spending more time providing informal educational activities; at minimum, caregiver mental health should be considered before turning informal educational activities over to volunteers.