Micrometer-scale maps of authigenic microstructures in submarine basaltic tuff specimens from a 1979 Surtsey volcano, Iceland, drill core acquired 15 years after eruptions terminated provide fresh perspectives for deciphering the initial alteration of oceanic basalt in a low temperature hydrothermal system. A novel investigative approach integrates synchrotron source X-ray microdiffraction (µXRD), X-ray microfluoresence (µXRF), micro-computed tomography (µCT), and scanning transmission electron microscopy (S/TEM) coupled with Raman spectroscopy to create finely resolved spatial frameworks that record a continuum of alteration in glass and olivine. Micro-analytical maps of vesicular and fractured lapilli in specimens from 157.1, 137.9, and 102.6 m depth, and borehole temperatures of 83, 93.9 and 141.3 °C measured in 1980, respectively, record the production of nanocrystalline clay mineral, zeolites, and Al-tobermorite in diverse microenvironments. Nanocrystalline clay mineral (nontronite) and zeolite (amicite) texture in linear microstructures have concentrically-oriented crystallographic preferred orientation. Raman spectra indicating degraded organic carbonaceous matter are associated with nanocrystalline clay mineral in 10–25 nm, sub-circular nanoscale cavities in altered glass at 137.9 m depth and in a concentrically-layered, crystallographically-oriented linear microstructure in altered olivine at 102.6 m. These features have little resemblance to previously described alteration features in basalt. Irregular alteration fronts between fresh and altered glass at 157.1 depth, however, show a resemblance to microchannels in older basalts. The integrated analyses describe the complex organization of previously unrecognized mineral textures in very young basalt and provide a foundational mineralogical reference for longitudinal, time-lapse characterizations of palagonitized basalt in oceanic environments.