In the vast research field on carbon nanostructures, a seemingly broadly accepted family configuration of nanoscale carbon allotropes is such that fullerenes take the zero-dimensional dot spot, in perfect harmony with one-dimensional carbon nanotubes and two-dimensional graphene nanosheets. More recently, however, a threat to the nice “family value” has been the emergence of small carbon nanoparticles, which are carbon particles of a few nanometers in size without any defined crystal structures or largely amorphous and populated with abundant surface and other defects. The growing experimental evidence has revealed the unique and/or advantageous optical and photoexcited state properties and photoinduced redox characteristics of the small carbon nanoparticles, elevating them to the position of being able to compete with fullerenes for the title of nanoscale carbon allotrope at the zero-dimension. Moreover, a related supporting argument is that fullerenes are molecules, nanoscale in their sizes but not necessarily “nanomaterials” strictly speaking. In this presentation, relevant experimental results of the nanoparticles and fullerenes will be compared for a fair assessment and judgment of their title competition, and more importantly their shared structural features and electronic properties and also their enormous potential in the development of materials for a variety of technological applications will be highlighted.