  In this paper, we investigate linear relations among regularized motivic
iterated integrals on $\mathbb{P}^{1}\setminus\{0,1,\infty\}$ of depth two,
which we call regularized motivic double zeta values. Some mysterious
connections between motivic multiple zeta values and modular forms are known,
e.g. Gangl--Kaneko--Zagier relation for the totally odd double zeta values and
Ihara--Takao relation for the depth graded motivic Lie algebra. In this paper,
we investigate so-called non-admissible cases and give many new
Gangl--Kaneko--Zagier type and Ihara--Takao type relations for regularized
motivic double zeta values. Specifically, we construct linear relations among a
certain family of regularized motivic double zeta values from odd period
polynomials of modular forms for the unique index two congruence subgroup of
the full modular group. This gives the first non trivial example of a
construction of the relations among multiple zeta values (or their analogues)
from modular forms for a congruence subgroup other than the ${\rm
SL}_{2}(\mathbb{Z})$.
