Background: In Romania, data regarding the oral health of infants and toddlers is scarce. This study aimed to analyze the reasons for the first dental visit among children aged 3 or under and to assess their oral health status and the therapeutic methods applied. Methods: A retrospective cross-sectional study was conducted on 602 children (339 boys and 263 girls), aged ≤ 3 years, who were referred for their first dental visit to the Pediatric Dentistry Department, Faculty of Dentistry, Carol Davila University, Bucharest, Romania. Results: The main reasons for referral were routine check-up (28.23%), asymptomatic carious lesions (21.92%), abscess or swelling (18.43%), and dental trauma (14.78%). Caries was diagnosed in 344 children; 23 (6.68%) had only non-cavitated lesions, 157 (45.64%) had uncomplicated cavitated lesions, and 174 (50.58%) already had complicated caries. Mean values of caries experience indices were significantly higher in rural children (dmf-t = 4.33 ± 4.13; dmf-s = 9.16 ± 11.34) than in urban children (dmf-t = 2.67 ± 3.61; dmf-s = 5.62 ± 8.86) (p = 0.000). The most frequent treatments were routine check-up with oral hygiene and dietary instructions (55.31%), pulp treatments (19.91%), and restorative procedures (15.1%). Conclusions: Many infants and toddlers were referred later than the recommended age and required therapeutic rather than preventive care. More than half had carious lesions, and many of those were already complicated. Significant disparities were observed between rural and urban children from this study group. Targeted public health initiatives are needed to improve early access to dental care.