Associations of cardiorespiratory fitness (CRF), physical activity (PA), sedentary behavior, and body fat percentage (BF%) with arterial stiffness and dilation capacity were investigated in 160 prepubertal children (83 girls) 6–8 years of age. We assessed CRF (watts/lean mass) by maximal cycle ergometer exercise test, total PA, structured exercise, unstructured PA, commuting to and from school, recess PA and total and screen-based sedentary behavior by questionnaire, BF% using dual-energy X-ray absorptiometry, and arterial stiffness and dilation capacity using pulse contour analysis. Data were adjusted for sex and age. Poorer CRF (standardized regression coefficient β = −0.297,P< 0.001), lower unstructured PA (β = −0.162,P= 0.042), and higher BF% (β = 0.176,P= 0.044) were related to higher arterial stiffness. When CRF, unstructured PA, and BF% were in the same model, only CRF was associated with arterial stiffness (β = −0.246,P= 0.006). Poorer CRF was also related to lower arterial dilation capacity (β = 0.316,P< 0.001). Children with low CRF (< median) and high BF% (≥ median;P= 0.002), low CRF and low unstructured PA (< median;P= 0.006) or children with low unstructured PA and high BF% (P= 0.005) had higher arterial stiffness than children in the opposite halves of these variables. Poor CRF was independently associated with increased arterial stiffness and impaired arterial dilation capacity among children.