Secondary ion mass spectrometry is an excellent technique of analytical chemistry, where primary ions sputter a solid sample generating the secondary ions which are determined. Although the ion yield is inherently low, it can be enhanced by using a post-ionization of sputtered neutral species. Our novel approach integrates this technique with a near infrared femtosecond laser post-ionization based on an adaptive control through a laser pulse shaper. The shaping of the laser pulse provides adaptive control to select a mass peak of interest and to enhance this peak intensity. Versatility is confirmed by optimizing the ion yield for different molecules (tryptophan, anthracene, polyethylene, and oxalic acid) with focus on parent ion enhancement, fragmentation process, sublimation effect, and excited secondary species. This proof-of-concept experiment provides not only a nonspecific increase of the overall ion yield, but also the selection of specific secondary species and the adaptive enhancement of their intensities on the order of 100, potentially simplifying data interpretation. Such tailored spectra might advance the (secondary ion) mass spectrometry to new capabilities.