Ground-based remote sensing using multi-axis differential optical absorption spectroscopy (MAX-DOAS) was used to conduct continuous simultaneous observations of ozone (O3), nitrogen dioxide (NO2), and formaldehyde (HCHO) concentrations at Chiba (35.63° N, 140.10° E, 21 m a.s.l.) and Tsukuba (36.06° N, 140.13° E, 35 m a.s.l.), Japan, for 7 years from 2013 to 2019. These are urban and suburban sites, respectively, in the greater Tokyo metropolitan area. NO2 and HCHO are considered to be proxies for nitrogen oxides (NOx) and volatile organic compounds (VOCs), respectively, both of which are major precursors of tropospheric O3. The mean concentrations below an altitude of 1 km were analyzed as planetary boundary layer (PBL) concentrations. For a more spatially representative analysis around the urban area of Chiba, four MAX-DOAS instruments directed at four different azimuth directions (north, east, west, and south) were operated simultaneously and their data were unified. During the 7-year period, the satellite observations indicated an abrupt decrease in the tropospheric NO2 concentration over East Asia, including China. This suggested that the transboundary transport of O3 originating from the Asian continent was likely suppressed or almost unchanged during the period. Over this time period, the MAX-DOAS observations revealed the presence of almost-constant annual variations in the PBL O3 concentration, whereas reductions in NO2 and HCHO concentrations occurred at rates of approximately 6–10%/year at Chiba. These changes provided clear observational evidence that a decreasing NOx concentration significantly reduced the amount of O3 quenched through NO titration under VOC-limited conditions in the urban area. Under the dominant VOC-limited conditions, the MAX-DOAS-derived concentration ratio of HCHO/NO2 was found to be below unity in all months. Thus, the multi-component observations from MAX-DOAS provided a unique data set of O3, NO2, and HCHO concentrations for analyzing PBL O3 variations.