Inferior coker gas oil (ICGO) derived from Venezuelan vacuum residue delayed coking is difficult to process using fluid catalytic cracking (FCC) or hydrocracking (HDC). The high content of nitrogen and condensed aromatics leads to major coking and readily deactivates the acid catalyst. In this work, a sequence of hydrotreating (HDT) and FCC processing is used to effectively convert ICGO to a high-value light oil product. The results show a higher overall conversion and a significant increase in the yield of gasoline compared to FCC processing. Molecular level characterization of the nitrogen compounds and condensed aromatics before and after HDT confirms that the nitrogen content and the 2+-ring aromatic content decreased, whereas the single-ring aromatics increased. The nitrogen compounds were mainly N-1, N1O1, N1O2, and N1S1 class species in basic nitrogen and N-1, N1O1, N1O2, N-2, and N2O1 class species in non-basic nitrogen. Moreover, the double bond equivalent of these species shifted to lower values. The decrease in the nitrogen compounds with a high heteroatom content reduces coking on the FCC catalyst. Subsequently, FCC unit performance and conversion to light oil increased. Moreover, the decrease in the size of N-1 class compounds and the ease of their cracking following HDT improved the performance of the FCC unit. Partial saturation of condensed aromatics following HDT also made it easier to crack these compounds.