Sole-source light-emitting diodes (LEDs) are alternatives to fluorescent tubes and high intensity discharge lamps that are routinely used for indoor cultivation of horticultural commodities, including microgreens. This study examined the effect of photosynthetic photon flux density (PPFD) from LEDs on phytochemical profiles of organically grown kale, cabbage, arugula, and mustard microgreens, and their association with growth and morphological attributes. LEDs were used to deliver a 15% blue light and 85% red light mixture to microgreens at varying PPFDs between 100 and 600 μmol·m⁻²·s⁻¹. For all microgreens, increased concentrations of ascorbate (total and reduced) and total anthocyanin were proportional to PPFD. Total phenolic concentrations were elevated in all four microgreens at high PPFDs, whereas chlorophyll concentrations declined in arugula, cabbage, and mustard. A principal component analysis revealed anthocyanins and phenolics were associated with ascorbate levels in all microgreens, but not with chlorophylls or carotenoids. At high PPFDs photosynthetic pigment levels were negatively associated with fresh and dry weight to varying degrees. Anthocyanins, phenolics, and ascorbate were negatively correlated with hypocotyl length and the colour attribute hue angle in all microgreens. These results indicate that microgreen growth and morphology are associated with altered phytochemical profiles during cultivation under sole-source LEDs.