Several polymer organic deposits (PODs) had been obtained by heating of nickel polyphosphate (NiP) at 720 K for 1, 4, or 10 h in a stream of helium (carrier gas) containing 20% of [ethylbenzene:oxygen=1:0.5] mixture. The samples were tested in oxidative dehydrogenation (OD) of ethylbenzene (EB) to styrene, before and after their separation from the inorganic part of NiP as catalysts. Some functional groups or bonds, important for enhancement of styrene yield, have been found in the PODs. The POD obtained after 10-h coking of NiP, containing a mixture of both insoluble fused-ring and soluble-in-pyridine macromolecules, provided with at least two types of catalytically active center, proved to be the most effective in EB OD.