In part 1 of this work, preparation, structure, spectroscopic, and electrochemical characteristics of the polypyrrole (PPy) deposited alumina/multi-walled carbon nanotubes (MWCNTs) inhibitor particles (PDAMIPs) are presented. TEM observations evidenced uniform deposition of thin PPy film on the functionalized nanotubes, whereas co-deposition of PPy and polystyrene sulfonic acid (PSS) lead to thick polymer coverage on hydrated alumina. Modification with polymer complexes resulted in moderately dispersed PDAMIPs, which is due to the various degrees of aggregation and coalescence. FTIR revealed compact and dense PPy structure on the functionalized MWCNTs while it was not the case on alumina and the PSS modified nanotubes. Closer interaction of PPy with the MWCNTs resulted in enhanced charge mobility, whereas greater electroactivity and reversibility of PPy were noted to samples containing functionalized nanotubes and low amount of PSS. Rheological study verified moderate micron-scale dispersity and the modification caused various degrees of aggregations of the PDAMIPs. These were recognized to be valid in the suspensions at a solid phase concentration with component contents similar to the corrosion tested hybrid coatings. Rheological percolation of the nanotubes (with anisotropic factor of ∼100) was confirmed at volume fractions of 3.30 × 10−3 and 6.0 × 10−4 which were under the dilute/semi-dilute boundary type theoretical and experimental thresholds. This is related to the extensive interconnection of the nanotube-supported filaments. Thus, overlapping of the nanotubes should contribute to the electrical percolation thereby galvanic corrosion prevention function of the zinc-rich hybrid coatings, which is discussed in the 2nd part.