Diastolic dysfunction (DD) commonly causes heart failure with preserved ejection fraction (EF). Here, we examine associations between DD severity and atherosclerosis/vascular calcification in hemodialysis patients. Echocardiography was performed on 101 patients undergoing hemodialysis therapy. Twelve patients (EF < 50% or chronic atrial fibrillation) were excluded; DD of the remaining 89 patients was classified into four grades. We then investigated the relationship between their DD grades and the cardio-ankle vascular index (CAVI), ankle-brachial pressure index (ABI), toe-brachial pressure index (TBI), and aortic calcification area index (ACAI). Seventy-seven patients (86.5%) with EF ≥ 50% had DD. Associations with advanced age and comorbid diabetes mellitus and cardiovascular disease were observed. The CAVI, TBI, and ACAI, but not ABI, increased proportionally with DD grades. Thus, many hemodialysis patients developed DD, with systolic function maintained. Strong associations between DD grades and progression of both atherosclerosis and vascular calcification could be inferred.