The molecular charge responses and bond-order changes due to the chemisorption are reported for model allyl-[MoO3] (010)-surface structures. Charge rearrangement patterns are determined from the charge sensitivity analysis (CSA) in the atomic resolution. The bond-order analysis is based upon the valence indices calculated within the one-determinantal (Kohn-Sham, KS) difference approach, comparing bonding patterns in a molecule and in the separated reactants limit, respectively. Polarization (P) and charge transfer (CT) stages of adsorption are examined separately; the overall (CT+P) patterns are also reported to examine the relative importance of these effects in the chemisorption systems considered. These charge sensitivity criteria are calculated from the semiempirical hardness matrix for M = (adsorbate/substrate) reactive systems including a large two-layer surface cluster. Rough estimates of the electrostatic (ES), P, and CT contributions to the interaction energy are also available in the CSA approach; they provide an approximate energetical hierarchy among the alternative chemisorption arrangements. These predictions are compared with the corresponding KS results for small surface clusters. The set of collective charge displacements, which diagonalize the interreactant part of the hardness matrix, are used to interpret the isoelectronic Fukui function for the allyl --> [MoO3] CT. The mechanism of selective allyl oxidation to acrolein is examined in more detail. It is shown that the selective allyl oxidation can be rationalized in a concerted bond-breaking-bond-forming mechanism, conjectured from a combination of the CSA charge rearrangements for large clusters and the KS bond multiplicity data for the smaller (active site) chemisorption complexes.