The dust-Hi correlation is used to characterize the emission properties of dust in the diffuse interstellar medium (ISM) from far infrared wavelengths to microwave frequencies. The field of this investigation encompasses the part of the southern sky best suited to study the cosmic infrared and microwave backgrounds. We present a general methodology to study the dust-Hi correlation over the sky, including simulations to quantify uncertainties. Our analysis yields four specific results. We analyse the residuals of the dust-Hi correlation. We identify a Galactic contribution to these residuals, which we model with variations of the dust emissivity on angular scales smaller than that of our correlation analysis. This model of the residuals is used to quantify uncertainties of the CIB power spectrum in a companion Planck paper.