Efficient production of nuclear isomers is critical for pioneering applications, like nuclear clocks, nuclear batteries, clean nuclear energy, and nuclear γ-ray lasers. However, due to small production cross sections and quick decays, it is extremely difficult to acquire a significant amount of isomers with short lifetimes via traditional accelerators or reactors because of low beam intensity. Here, for the first time, we experimentally present femtosecond pumping of nuclear isomeric states by the Coulomb excitation of ions with the quivering electrons induced by laser fields. Nuclei populated on the third excited state of ^{83}Kr are generated with a peak efficiency of 2.34×10^{15} particles/s from a tabletop hundred-TW laser system. It can be explained by the Coulomb excitation of ions with the quivering electrons during the interaction between laser pulses and clusters at nearly solid densities. This efficient and universal production method can be widely used for pumping isotopes with excited state lifetimes down to picoseconds, and could be a benefit for fields like nuclear transition mechanisms and nuclear γ-ray lasers.