We sought to describe and explore relationships between fundamental movement skills (FMS) and level of physical activity (PA; light-, medium-, vigorous, and kCal/hour) in preschool children, aged 3–4-years-old, across four early childhood education (ECE) settings. Children’s FMS were assessed using the Test for Gross Motor Development-2 (TGMD-2; n = 81) and PA via accelerometers (S = 53). Eighty-four children participated, with 50 in both assessments. The TGMD-2 showed as the children got older, their locomotor skills (p < 0.001, r = 0.512) and object control motor skills (p < 0.001, r = 0.383) improved. Accelerometry showed children were primarily inactive at ECE (78.3% of the time). There were significant correlations between kCal/hour and light (p < 0.001, r = −0.688), moderate (p < 0.001, r = 0.599) and vigorous (p < 0.001, rs = 0.707) activity, and between gross motor quotient and locomotor (p < 0.001, r = 0.798) and object control (p < 0.001, r = 0.367) skills. No correlation was observed between gross motor quotient and kCal/hour. To conclude, children in this cohort were primarily inactive during ECE center hours. Moreover, gross motor quotient was significantly correlated to locomotor and object control skills.