Biochemical markers of cartilage and bone degradation are becoming increasingly important in the evaluation of knee osteoarthritis (OA). To clarify the correlation between radiological knee OA and urine CTX-II (C-terminal crosslinking telopeptide of collagen type II) or urine NTX-I (N-terminal crosslinking telopeptide of type I collagen), we conducted a cross-sectional study in the cohorts of the epidemiological knee survey at the Matsudai district in Niigata Prefecture, Japan. Urine specimens were collected from 296 subjects, and CTX-II and NTX-I were measured using ELISA. Standing knee AP X-rays were obtained and graded according to the Kellgren-Lawrence classification. The subjects were then divided by gender, age (40- to 59-year-old group and 60- to 79-year-old group), and the X-ray grade (Grade 0, 1, Grade 2, and Grade 3, 4). In non-OA (Grade 0, 1) subjects, the 60- to 79-year-old group had significantly higher CTX-II values than the younger group only in females. The subjects of both genders aged over 60 years of age with OA Grade 3, 4 had significantly higher CTX-II values than the Grade 0, 1 group or the Grade 2 group. For NTX-I, there were no significant differences between each OA grade although the Grade 3, 4 group females from 60 to 79 years of age had higher values than the Grade 2 group. In addition, in the 60- to 79-year-old subjects of both genders, a positive correlation was observed between the urine CTX-II and urine NTX-I. For the subjects ranging from 60 to 79 years of age in both genders, the urine CTX-II values indicate the progression of OA. In addition, the weak but positive correlation between urine CTX-II and urine NTX-I in the subjects ranging from 60 to 79 years of age in both genders suggests that bone resorption and cartilage degradation appear to develop in parallel.