The ability to design and control
the chemical characteristics
of covalent organic frameworks (COFs) offers a new avenue for the
development of functional materials, especially with respect to topological
properties. Based on density functional theory calculations, by varying
the core units through the choice of bridging groups [O, CO,
CH2, or C(CH3)2] and the linker units
[acetylene, diacetylene, or benzene], we have designed heterotriangulene-based
COFs that are predicted to be two-dimensional higher-order topological
insulators (TIs). The higher-order TI characteristics of these COFs
are identified via their topological invariants and the presence of
in-gap topological corner modes and gapped edge states. The frontier
molecular orbital energies of the building moieties play an important
role in determining the size of the higher-order TI gap, which we
find to be highly dependent on linker units. We also examined the
deposition of the COFs on a boron nitride substrate to assess the
feasibility of experimental observation of a higher-order TI phase
in the organic layer. This work thus provides new insights into heterotriangulene-based
COFs and guidance for the exploration of purely organic topological
materials.