In the Maastrichtian-Danian chalk in the North Sea, discrete intervals, appearing as normal white chalk, contain up to 60% α-quartz <2 μm in size. Atomic force microscopy (AFM) reveals that the particles are of nm size, appearing as spherical particles and aggregates. Similar particles consisting of opal-CT were found in surface exposures of chalk in Denmark. Two new abiogenic pathways of silica formation in chalk are proposed. The first model proposes that SiO2 nano-size particles and aggregates precipitated and flocculated in the free-water phase as opal and were diagenetically transformed from opal-CT at low temperature to α-quartz at elevated temperature. In the second model, the dominance of radiolarians in the deep-water environment of the North Sea resulted in low dissolution supply with subsequent precipitation and flocculation of nano-size α-quartz particles. In the shallower water of the shelf environment of the present onshore chalk, the abundance of sponges and their dissolution supplied enough Si to precipitate opal-CT in the free-water phase.