A new method of using the detonation nanodiamond with positive and negative zeta potential as a spacer for aerogels based on graphene oxide is presented. It is shown that the dosed addition of detonation nanodiamonds’ particles to the suspension of graphene oxide hydrosol made it possible to triple the specific surface area of the resulting aerogel compared to graphene oxide aerogel, and this effect is more significant when nanodiamonds with a positive zeta potential are used. It was also shown that aerogels derived from graphene oxide and detonation nanodiamond with a positive zeta potential have a specific morphology with graphene oxide platelets being twisted. This effect is discussed in terms of the change in the average zeta potential of the initial mixtures.