The β-carotene and annatto extract are typical carotenoids used as a safe colorant of foods. However, the instability against irradiation limits their wide use. The improvement of the stability was investigated by the intercalation of the dye into the interlayer space of the anion-exchangeable clay, hydrotalcite. The hydrophobic environment was constructed in the interlayer space of the hydrotalcite by the modification with anionic surfactant (dodecyl sulfate and dodecylbenzene sulfonate). The lipophilic β-carotene and annatto dye were successfully incorporated into the organo-modified hydrotalcite, and the incorporated dye exhibited the improved photostability under visible irradiation from a 100 W halogen lamp (190 klux) in the air. The effect of the stabilization on the anionic annatto dye was higher by the incorporation in the modified hydrotalcite than in the modified cation exchangeable clay, suggesting that the polarity of the clay sheet had some influence on the stabilization of the incorporated dye. The stabilization effect of the β-carotene was not so significant as that of the annatto dye, because sufficient intercalation of the non-polar β-carotene may require stronger hydrophobic environment. The π-π interaction between the β-carotene and the benzene ring of the dodecylbenzene sulfonate was found to contribute to the stability enhancement.