From 2017 to 2019, an extensive sampling campaign was conducted in Belgian inland and coastal waters, aimed at providing paired data of optical and biogeochemical properties to support research into optical monitoring of aquatic systems. The campaign was focused on inland waters, with sampling of four lakes and a coastal lagoon during the growth season, in addition to samples of opportunity from other four lakes. Campaigns also included the Scheldt estuary over a tidal cycle and two sampling campaigns in the Belgian coastal zone. Measured parameters include inherent optical properties (absorption, scattering and beam attenuation coefficients, near-forward volume scattering function, turbidity), apparent optical properties (Secchi disc depth, substrate and water-leaving Lambert-equivalent bi-hemispherical reflectance), and biogeochemical properties (suspended particulate matter, mineral fraction of particle mass, particle size distribution, pigment concentration, DNA metabarcoding, flow microscopy counts, and bottom type classification). The diversity of water bodies and environmental conditions covered a wide range of system states. The chlorophyll a concentration varied from 0.63 to 382.72 mg m−3, while the suspended particulate matter concentration varied from 1.02 to 791.19 g m−3, with mineral fraction varying from 0 to 0.95. Depending on system and season, phytoplankton assemblages were dominated by cyanobacteria, green algae (Mamiellophyceae, Pyramimonadophyceae), or diatoms.