The objective of this study was to identify the major socio-demographic, health, and environmental determinants of stunting among children aged 0–59 months from the Tete province (Mozambique) and offering useful information for future healthcare strategies and interventions. A case-control study was conducted among 282 (162 boys; 120 girls) children under five years of age from the central region of Mozambique between 1 May and 3 June 2014. Children with stunting (HAZ < −2 SD according to the WHO Child Growth Standards in 2006) were considered as cases and those who had a Z-score < −2 SD were considered as controls. We collected data related to mothers and children and their environment, and they were assessed in two groups to find a possible association. The software used for data analysis was the SPSS® (version, 21.0) using descriptive statistics, t-test, ANOVA, chi-square analyses, bivariate comparisons, and stepwise multiple logistic regression analysis. The results showed that birth weight, mother’s educational status, maternal occupation, living in a rural area, family size, number of children under five years of age in the household, cooking with charcoal, inhabiting wooden or straw housing or housing without proper floors, overall duration of breastfeeding as well as duration of exclusive breastfeeding, and time of initiation of complementary feeding were significantly related to stunting. Thus, appropriate nutritional intervention programmes considering these determinants and the dissemination of knowledge at the population level related to undernutrition are necessary to ameliorate the children´s nutritional status.