  Parity- and time reversal-violating (PVTV) pion-nucleon couplings govern the
magnitude of long-range contributions to nucleon and atomic electric dipole
moments. When these couplings arise from chiral symmetry-breaking CP-violating
operators, such as the QCD $\theta$-term or quark chromoelectric dipole
moments, one may relate hadronic matrix elements entering the PVTV couplings to
nucleon and pion mass shifts by exploiting the corresponding chiral
transformation properties at leading order (LO) in the chiral expansion. We
compute the higher-order contributions to the lowest order relations arising
from chiral loops and next-to-next-to leading order (NNLO) operators. We find
that for the QCD $\theta$-term the higher order contributions are analytic in
the quark masses, while for the quark chromoelectric dipole moments and chiral
symmetry-breaking four-quark operators, the matching relations also receive
non-analytic corrections. Numerical estimates suggest that for the isoscalar
PVTV pion-nucleon coupling, the higher order corrections may be as large as
$\sim 20\%$, while for the isovector coupling, more substantial corrections are
possible.
