As the focus of integration technology inevitably shifts from the present very large scale integration (VLSI) to ultra large scale integration (ULSI) schemes, thus leading to continuous decrease in circuit dimensions, the limitations of present multilevel metallization technologies become increasingly important. Because of the appreciably higher speeds and more complex multi-functional layering involved in the newest ULSI circuits, the electrical resistance and capacitance of presently used interconnects and their electromigration and stress resistance stand as major limiting factors to signal processing throughput. In this paper, some recent results achieved by the present investigators in their studies of blanket and selective low-temperature metal-organic chemical vapor deposition (LTMOCVD) of copper for potential use in multilevel metallizations in ULSIC’s are presented. The films were produced at 300–400°C in atmospheres of pure H2 or Ar from the β-diketonate precursor bis(6, 6, 7,7, 8, 8, 8-heptafluoro-2, 2-dimethy1-3, 5-octanediono)copper(II), Cu(fod)2. The films were analyzed by x-ray diffraction (XRD), Rutherford Backscattering (RBS), Auger electron spectroscopy (AES), scanning electron microscopy (SEM), energy-dispersive x-ray spectroscopy (EDXS), and four-point resistivity probe. The results of these studies showed that films deposited on metallic substrates were uniform, continuous, adherent, highly pure, and exhibited very low resistivity, as low as 1.8 μΩcm for films deposited in pure H2 atmosphere. Preliminary investigations of selective LTMOCVD of copper showed that selectivity is indeed possible, but is a function of a wide range of parameters that include reactor geometry, substrate type and temperature, working pressure, type of carrier gas, and precursor chemistry.