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We propose observations of the H2 pure rotational transitions in the ultraluminous galaxies/quasars Arp 220, Mrk 231, FSC10214+4724, and H1413+117 in order to probe the warm molecular gas content in these extraordinarily gas-rich systems. In Arp 220 and Mrk 231, the S0 (28um),S1 (17um), and S3 (9.7um) transitions will be observed; in the two high redshift systems only the S1 and S3 lines are proposed. Detection of these transitions with ISO should be possible if significant fractions (ranging between 0.0001 and 0.1) of the total molecular gas contents are at temperatures exceeding 200-400 K. While these conditions would be very exceptional for the molecular clouds in normal galaxies, they may not be unreasonable for these rapidly evolving systems with extraordinarily high radiation densities. The detection of the H2 pure rotational transitions with ISO will imply that the gas in the high luminosity galaxies is much hotter (>200K), requiring a very critical re-evalution of the mm-wave line analysis.