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Amongst the problems facing South Africa today are malnutrition and food insecurity, and there is a need for interventions and innovative strategies to address these. The aim of the study was to determine the contribution of caregivers’ knowledge of nutrition and household food security among children aged 0 to 60 months. A cross-sectional study design was applied using a quantitative approach. A convenience sample (n = 184) of caregiver–child pairs (for children 0 to 60 months) from the Dora Nginza Hospital Paediatric Outpatient Department was used. A structured questionnaire was applied to collect data on socio-economic factors, health status, household food security, and caregivers’ knowledge. In addition, interviews were conducted, and anthropometric measurements of children were taken to determine their nutritional status. The results indicate that most caregivers were female, and more than half completed high school, yet almost 75% were unemployed. Most of the caregivers (58.2%) were either overweight or obese. The results also show that only 33.2% of households were food secure, 29.3% were at risk of hunger, and 37.5% experienced hunger. The prevalence of stunting, underweight, and wasting among children in the study was high. A significant, slightly positive correlation was found between the body mass index of the caregiver and height for age. Poor socio-economic status and food inaccessibility were identified as possible underlying contributing factors to malnutrition, contributing to food insecurity and therefore poor dietary intake.