Agates in Paleocene/Eocene tuffs from El Picado/Los Indios, Cuba were investigated to characterize the mineral composition of the agates and to provide data for the reconstruction of agate forming processes. The volcanic host rocks are strongly altered and fractured and contain numerous fissures and veins mineralized by quartz and chalcedony. These features indicate secondary alteration and silicification processes during tectonic activities that may have also resulted in the formation of massive agates. Local accumulation of manganese oxides/hydroxides, as well as uranium (uranyl-silicate complexes), in the agates confirm their contemporaneous supply with SiO2 and the origin of the silica-bearing solutions from the alteration processes. The mineral composition of the agates is characterized by abnormal high bulk contents of opal-CT (>6 wt%) and moganite (>16 wt%) besides alpha-quartz. The presence of these elevated amounts of “immature” silica phases emphasize that agate formation runs through several structural states of SiO2 with amorphous silica as the first solid phase. A remarkable feature of the agates is a heterogeneous distribution of moganite within the silica matrix revealed by micro-Raman mapping. The intensity ratio of the main symmetric stretching-bending vibrations (A1 modes) of alpha-quartz at 465 cm−1 and moganite at 502 cm−1, respectively, was used to depict the abundance of moganite in the silica matrix. The zoned distribution of moganite and variations in the microtexture and porosity of the agates indicate a multi-phase deposition of SiO2 under varying physico-chemical conditions and a discontinuous silica supply