As part of a large study to investigate the nature of the longer wavelength continuum emission of radio-loud AGN, we present new mid to far-infrared (MFIR) and high frequency radio observations for a complete sample of 2Jy powerful, southern radio galaxies at intermediate redshifts (0.05<z<0.7). Utilizing the sensitivity of the Spitzer Space Telescope, we have made deep MIPS observations at the wavelengths of 24, 70 and 160 microns, detecting 100% of our sample at 24 microns, and 90% at 70

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... ns. This high detection rate at MFIR wavelengths is unparallelled in samples of intermediate redshift radio galaxies. Complementing these results, we also present new high frequency observations (15 to 24Ghz) from the Australia Telescope Compact Array (ATCA) and the Very Large Array (VLA), which are used to investigate the potential contamination of the MFIR continuum by non-thermal synchrotron emission. With the latter observations we detect the compact cores in 59% of our complete sample, and deduce that non-thermal contamination of the MFIR continuum is significant in a maximum of 30% of our total sample. MFIR fluxes, radio fluxes and spectral energy distributions for the complete sample are presented here, while in a second paper we will analyse these data and discuss the implications for our understanding of the heating mechanism for the warm/cool dust, star formation in the host galaxies, and the unified schemes for powerful radio sources.