The sorption behavior and spatial microdistribution of Cs-137, Sr-90 and Am-241 onto the surface of a fractured rock sample from the R-11 borehole of the exocontact zone of the Nizhnekansky granitoid massif were studied. The sorption efficiency of the fractured sample increases in the row of Sr < Cs < Am, where americium is the most retained radionuclide. Based on the image processing of radiograms and scanning electron microscopy data, the mineral relative sorption efficiency (RSE) values were determined to quantify the contribution of the mineral phases of the fractured sample to radionuclide retention. It was established that cesium and strontium are predominantly retained in cracks filled with secondary mineral chlorite. Zeolite is a less effective sorbent with respect to cesium and strontium. Americium sorption is uniform over the whole surface of the fractured sample, with close RSE values for all mineral phases (RSE ~1). The behavior of cesium in heterogeneous and monomineral systems of crushed mineral phases of quartz, biotite and zeolite NaA imitating minerals of the fractured rock sample R-11 was determined. It was shown that the fraction of the sorbed cesium in a heterogeneous system of two mineral phases—biotite and quartz—was larger than the sum of sorption values for the same separated mineral phases. Based on the models of radionuclide sorption on illite–smectite minerals, it was able to estimate the depth of the penetration of solution into the fractured rock sample R-11. The variations of penetration depths for solutions of specific radionuclide into the fractured rock sample were established.