The Fukushima Daiichi accident resulted in the release of a novel form of radioactive Cs contamination into the environment, called Cs-bearing microparticles (CsMP). CsMPs constitute a substantial portion of the radioactive pollution near the nuclear power station and traveled beyond several hundred kilometers. Extensive characterization of the CsMPs revealed an amorphous silica matrix, along with Cs and other minor or trace elements such as Fe and Zn. This study explores the unclear generation mechanism of CsMPs by conducting experimental molten core concrete interactions (MCCI) as a source of Si and analyzing the resultant aerosols. The findings demonstrate that MCCI is in capacity to produce spherical submicronic and micronic particles, primarily composed of amorphous silica and incorporating elements akin to CsMPs. A humid atmosphere is found to favour an even closer chemical composition. Examination of the internal structure of the synthesized particles unveils numerous crystalline nanoinclusions, similar to those observed in CsMPs, possibly serving as nucleation sites for CsMP formation through the condensation of Si-rich vapors.