Nanoporous silica zeolite thin films are promising candidates for future generation low-dielectric constant (low-k) materials. During the integration with metal interconnects, residual stresses resulting from the packaging processes may cause the low-k thin films to fracture or delaminate from the substrates. To achieve high-quality low-k zeolite thin films, it is important to carefully evaluate their adhesion performance. In this paper, a previously reported laser spallation technique is modified to investigate the interfacial adhesion of zeolite thin film-Si substrate interfaces fabricated using three different methods: spin-on, seeded growth, and in situ growth. The experimental results reported here show that seeded growth generates films with the highest measured adhesion strength (801 ± 68 MPa), followed by the in situ growth (324 ± 17 MPa), then by the spin-on (111 ± 29 MPa). The influence of the deposition method on film–substrate adhesion is discussed. This is the first time that the interfacial strength of zeolite thin films-Si substrates has been quantitatively evaluated. This paper is of great significance for the future applications of low-k zeolite thin film materials.