Following our previous works on pure-silica-zeolite (PSZ) MFI, in this study we explore PSZ MEL as a new option for low-k dielectric films. Our motivation has been to increase the microporosity of the spin-on films by moving to structures with a framework density (FD) lower than MFI. Nanoparticle PSZ MEL suspensions were synthesized by a two-stage method that allowed the yield of nanocrystals to be significantly enhanced, while the zeolite nanocrystals remain small. For the first time zeolite nanocrystals of about 50 nm were synthesized with a yield as high as 57%. Nanoparticle suspensions with different particle sizes and crystallinities were spun on silicon wafers to prepare continuous thin films. An ultralow-k value as low as 1.5 was obtained with MEL nanoparticle suspension of high relative crystallinity. The surface roughness of the PSZ MEL film with high relative crystallinity is greatly improved (R(rms) approximately 5.6 nm) compared to MFI films with high relative crystallinity (R(rms) approximately 12 nm).