I found
$$\sum_{n=1}^\infty\frac{2^{2n}H_n}{n^3{2n\choose n}}=-8\int_0^{\pi/2}x^2\cot x\ln(\cos x)\ dx=I\tag1.$$
Mathematica failed to find $I$, so I am not sure if there is closed form for it. I am just giving it a try here.
First idea came to my mind is to use the Fourier series of $-\ln(\cos x)=\ln(2)+\sum_{n=1}^\infty\frac{(-1)^n\cos(2nx)}{n}$ and we have
$$I=8\ln(2)\underbrace{\int_0^{\pi/2}x^2\cot x\ dx}_{\frac32\ln(2)\zeta(2)-\frac78\zeta(3)}+8\sum_{n=1}^\infty\frac{(-1)^n}{n}\int_0^{\pi/2}x^2 \cot x\cos(2nx)\ dx.$$
I got stuck here. Any help would be much appreciated.
Proof of $(1)$
from here we have
$$\arcsin^2(x)=\frac12\sum_{n=1}^\infty\frac{(2x)^{2n}}{n^2{2n\choose n}}$$
replace $x$ by $\sqrt{x}$ we get $$\sum_{n=1}^\infty\frac{2^{2n}x^n}{n^2{2n\choose n}}=2\arcsin^2(\sqrt{x})$$
multiply both sides by $-\frac{\ln(1-x)}{x}$ then $\int_0^1$ and use $-\int_0^1 x^{n-1}\ln(1-x)dx=\frac{H_n}{n}$ we get
$$\sum_{n=1}^\infty\frac{2^{2n}H_n}{n^3{2n\choose n}}=2\int_0^1\frac{\arcsin^2(\sqrt{x})\ln(1-x)}{x}dx\overset{\sqrt{x}=\sin\theta}{=}-8\int_0^{\pi/2}x^2\cot x\ln(\cos x)\ dx$$
Thanks to @user97357329 for his hint in the comments.
In the book, Almost Impossible Integrals, Sums and Series, page $247$ Eq $(3.288)$ we have
$$\cot x\ln(\cos x)=\sum_{n=1}^\infty(-1)^n\left(\psi\left(\frac{n+1}{2}\right)-\psi\left(\frac{n}{2}\right)-\frac1n\right)\sin(2nx)$$
$$=\sum_{n=1}^\infty(-1)^n\left(\int_0^1\frac{1-t}{1+t}t^{n-1}dt\right)\sin(2nx),\quad 0<x<\frac{\pi}{2}$$
Thus,
$$\int_0^{\pi/2}x^2\cot x\ln(\cos x)dx=\sum_{n=1}^\infty(-1)^n\left(\int_0^1\frac{1-t}{1+t}t^{n-1}dt\right)\left(\int_0^{\pi/2}x^2\sin(2nx)dx\right)$$
$$=\sum_{n=1}^\infty(-1)^n\left(\int_0^1\frac{1-t}{1+t}t^{n-1}dt\right)\left(\frac{\cos(n\pi)}{4n^3}-\frac{3\zeta(2)\cos(n\pi)}{4n}-\frac{1}{4n^3}\right)$$
$$=\sum_{n=1}^\infty(-1)^n\left(\int_0^1\frac{1-t}{1+t}t^{n-1}dt\right)\left(\frac{(-1)^n}{4n^3}-\frac{3\zeta(2)(-1)^n}{4n}-\frac{1}{4n^3}\right)$$
$$=\frac14\int_0^1\frac{1-t}{t(1+t)}\left(\sum_{n=1}^\infty\frac{t^n}{n^3}-\frac{3\zeta(2)t^n}{n}-\frac{(-t)^n}{n^3}\right)dt$$
$$=\frac14\int_0^1\left(\frac1t-\frac2{1+t}\right)\left(\text{Li}_3(t)+3\zeta(2)\ln(1-t)-\text{Li}_3(-t)\right)dt$$
$$=\frac14\underbrace{\int_0^1\frac{\text{Li}_3(t)-\text{Li}_3(-t)}{t}dt}_{\mathcal{I}_1}-\frac12\underbrace{\int_0^1\frac{\text{Li}_3(t)-\text{Li}_3(-t)}{1+t}dt}_{\mathcal{I}_2}$$ $$+\frac34\zeta(2)\underbrace{\int_0^1\frac{\ln(1-t)}{t}dt}_{\mathcal{I}_3}-\frac32\zeta(2)\underbrace{\int_0^1\frac{\ln(1-t)}{1+t}dt}_{\mathcal{I}_4}$$
$$\mathcal{I}_1=\text{Li}_4(1)-\text{Li}_4(-1)=\zeta(4)+\frac78\zeta(4)=\boxed{\frac{15}{8}\zeta(4)}$$
By integration by parts we have
$$\mathcal{I}_2=\frac74\ln(2)\zeta(3)-\int_0^1\frac{\ln(1+t)\text{Li}_2(t)}{t}dt+\int_0^1\frac{\ln(1+t)\text{Li}_2(-t)}{t}dt$$
$$=\frac74\ln(2)\zeta(3)+\sum_{n=1}^\infty\frac{(-1)^n}{n}\int_0^1 t^{n-1}\text{Li}_2(t)dt-\frac12\text{Li}_2^2(-t)|_0^1$$
$$=\frac74\ln(2)\zeta(3)+\sum_{n=1}^\infty\frac{(-1)^n}{n} \left(\frac{\zeta(2)}{n}-\frac{H_n}{n^2}\right)-\frac5{16}\zeta(4)$$ $$=\frac74\ln(2)\zeta(3)-\frac54\zeta(4)-\sum_{n=1}^\infty\frac{(-1)^nH_n}{n^3}-\frac5{16}\zeta(4)$$ substitute
$$\sum_{n=1}^\infty\frac{(-1)^nH_n}{n^3}=2\operatorname{Li_4}\left(\frac12\right)-\frac{11}4\zeta(4)+\frac74\ln2\zeta(3)-\frac12\ln^22\zeta(2)+\frac{1}{12}\ln^42$$
we get
$$\mathcal{I}_2=\boxed{-2\operatorname{Li_4}\left(\frac12\right)-\frac{25}{16}\zeta(4)+\frac12\ln^22\zeta(2)-\frac{1}{12}\ln^42}$$
$$\mathcal{I}_3=-\text{Li}_2(1)=\boxed{-\zeta(2)}$$
$$\mathcal{I}_4=\int_0^1\frac{\ln(1-t)}{1+t}dt=\int_0^1\frac{\ln x}{2-x}dx=\sum_{n=1}^\infty\frac1{2^n}\int_0^1 x^{n-1}\ln xdx$$ $$=-\sum_{n=1}^\infty\frac{1}{n^22^n}=-\text{Li}_2\left(\frac12\right)=\boxed{\frac12\ln^22-\frac12\zeta(2)}$$
Combine all boxed results we finally get
$$\int_0^{\pi/2}x^2\cot x\ln(\cos x)dx=\text{Li}_4\left(\frac12\right)-\frac18\zeta(4)-\ln^2(2)\zeta(2)+\frac{1}{24}\ln^4(2)$$
which gives us
$$\sum_{n=1}^\infty\frac{2^{2n}H_n}{n^3{2n\choose n}}=-8\text{Li}_4\left(\frac12\right)+\zeta(4)+8\ln^2(2)\zeta(2)-\frac{1}{3}\ln^4(2)$$