Background: Diarrheal disease is among the leading causes of death in children younger than 5 years, especially in developing countries. The aim of this study was to investigate the most frequent etiological agents of diarrhea and its associated factors in children younger than 5 years attending the Bengo General Hospital in Angola. Methods: From September 2012 through December 2013, stool samples were collected from 344 children presenting with diarrhea to investigate the presence of viral, bacterial and parasitic agents. Relevant sociodemographic and clinical data were obtained from parents and caregivers. Results: An enteric pathogen was detected in 66.6% of stool samples: Cryptosporidium spp. (30.0%), rotavirus (25.1%), Giardia lamblia (21.6%), diarrheagenic Escherichia coli (6.3%), Ascaris lumbricoides (4.1%), adenovirus (3.8%), Strongyloides stercoralis (3.5%), astrovirus (2.6%), Hymenolepis nana (1.7%), Entamoeba histolytica/dispar (0.9%), Taenia spp. (0.6%), Trichuris trichiura (0.3%) and Entamoeba histolytica (0.3%). Children younger than 12 months were more frequently infected with Cryptosporidium spp. compared with older children (age: 12-59 months), independently of sex, season, lethargy and wasting [odds ratio (OR): 3.5, 95% confidence interval (95% CI): 2.0-6.2]. Age (OR: 5.0, 95% CI: 2.6-9.3), vomiting (OR: 2.7, 95% CI: 1.5-4.8) and type of admission (inpatients, OR: 0.5, 95% CI: 0.3-0.9) were significantly associated with rotavirus infection. Conclusions: This study demonstrates high rates of infection with an enteric pathogen, particularly in children younger than 12 months, emphasizing the need to address diarrheal disease in this age group.