Note that by symmetry, for the double cone to split the sphere into two pieces of equal volume, each hemisphere must also be split into two pieces of equal volume by each cone. So we can just work with the upper hemisphere. Since a sphere has volume $\displaystyle\frac{4\pi r^{3}}{3}$, the volume a hemisphere is $\displaystyle\frac{2\pi r^{3}}{3}$.
Using standard spherical coordinates $(\theta,\phi,\rho)$, the equation of the sphere is $\rho=r$ and the equation of the cone is $\phi=\phi_{0}$, where $\phi_{0}\in[0,\pi/2]$ is the desired angle. We can then easily compute the volume of the sphere below the cone:
\begin{align}
V &= \int_{0}^{2\pi}\int_{0}^{\phi_{0}}\int_{0}^{r}\rho^{2}\sin{\phi}\ d\rho\ d\phi \ d\theta\\
&=\frac{r^{3}}{3}\int_{0}^{2\pi}\left(-\cos{\phi}\bigg\rvert^{\phi_{0}}_{0}\right)\ d\theta \\
&= \frac{2\pi r^{3}}{3}(-\cos{\phi_{0}}+1)
\end{align}
Now, we want this volume to be half of the volume of the hemisphere, so we should have
$$\frac{2\pi r^{3}}{3}(-\cos{\phi_{0}}+1)=\frac{\pi r^{3}}{3}$$
which yields
$$\cos{\phi_{0}}=\frac{1}{2}$$
so the desired angle is
$$\phi_{0}=\cos^{-1}\left(\frac{1}{2}\right)=\frac{\pi}{3}$$ I should mention that this angle $\phi$ is measured from the top of the $z$-axis.