Green authigenic mica, i.e., celadonite, is commonly associated with submarine alteration of basic igneous rock. However, very few studies have reported the formation of celadonite under nonmarine conditions. An integrated study involving field investigation, petrography, mineralogy, and mineral chemistry highlighted the origin of celadonite in two clay-rich horizons (green boles) of the Late Cretaceous Deccan volcanic province. Within the Salher green bole, the celadonite occurred as the dissolution and alteration of plagioclase, volcanic glass, and pore-filling cement. In the case of the Pune green bole, the celadonite was formed by the alteration of plagioclase, pyroxene, and precipitation as film within intergranular pores, along with zeolite. The celadonite in the Salher green bole exhibited slightly lower K2O and Fe2O3 and higher Al2O3 than in the Pune. The mineral chemistry of the former showed a composition closer to ferro-aluminoceladonite. Although the mineral chemistry of celadonite overlaps with glauconite, the distinct 10 Å and 15 Å reflections in XRD, euhedral lath and honeycomb morphology under SEM, and characteristic absorption bands in VNIR spectroscopy (0.4–2.5 µm) and FTIR spectroscopy (400–4000 cm−1) identified celadonite and Fe-smectite within green boles. The green boles were formed either by the alteration of a volcaniclastic deposit in local pools of water or by the in situ alteration of the fragmentary flow top. The present study is significant due to the occurrence of celadonite in a nonmarine environment, as it otherwise forms under submarine conditions.