By way of enrichment here is another algebraic proof using basic
complex variables, quite similar to the accepted answer.
Note that the second binomial coefficient in both sums controls the
range of the sum, so we can write our claim like this:
$$\sum_{k=0}^{n+1} {n+1\choose k} (-1)^k {2n-3k\choose n-3k}
= \sum_{k=0}^{n+1} {n+1\choose k} {k\choose n-k}.$$
To evaluate the LHS introduce the integral representation
$${2n-3k\choose n-3k} =
\frac{1}{2\pi i}
\int_{|z|=\epsilon}
\frac{(1+z)^{2n-3k}}{z^{n-3k+1}} \; dz.$$
We can check that this really is zero when $k>\lfloor n/3\rfloor.$
This gives for the sum the representation
$$\frac{1}{2\pi i}
\int_{|z|=\epsilon}
\frac{(1+z)^{2n}}{z^{n+1}}
\sum_{k=0}^{n+1} {n+1\choose k}
(-1)^k \left(\frac{z^3}{(1+z)^3}\right)^k
\; dz
\\ = \frac{1}{2\pi i}
\int_{|z|=\epsilon}
\frac{(1+z)^{2n}}{z^{n+1}}
\left(1-\frac{z^3}{(1+z)^3}\right)^{n+1} \; dz
\\ = \frac{1}{2\pi i}
\int_{|z|=\epsilon}
\frac{1}{z^{n+1}} \frac{1}{(1+z)^{n+3}}
\left(3z^2+3z+1\right)^{n+1} \; dz
\\ = \frac{1}{2\pi i}
\int_{|z|=\epsilon}
\frac{1}{z^{n+1}} \frac{1}{(1+z)^{n+3}}
\sum_{q=0}^{n+1} {n+1\choose q} 3^q z^q (1+z)^q \; dz
\\ = \frac{1}{2\pi i}
\int_{|z|=\epsilon}
\sum_{q=0}^{n+1} {n+1\choose q} 3^q z^{q-n-1} (1+z)^{q-n-3} \; dz
\\ = \frac{1}{2\pi i}
\int_{|z|=\epsilon}
\sum_{q=0}^{n+1} {n+1\choose q} 3^q
\frac{1}{z^{n+1-q}} \frac{1}{(1+z)^{n+3-q}} \; dz.$$
Computing the residue we find
$$\sum_{q=0}^{n+1} {n+1\choose q} 3^q (-1)^{n-q}
{n-q+n+2-q\choose n+2-q}
= \sum_{q=0}^{n+1} {n+1\choose q} 3^q (-1)^{n-q}
{2n-2q+2\choose n-q+2}.$$
Now introduce the integral representation
$${2n-2q+2\choose n-q+2}
= \frac{1}{2\pi i}
\int_{|z|=\epsilon}
\frac{(1+z)^{2n-2q+2}}{z^{n-q+3}} \; dz$$
which gives for the sum the integral
$$\frac{1}{2\pi i}
\int_{|z|=\epsilon}
\frac{(1+z)^{2n+2}}{z^{n+3}}
\sum_{q=0}^{n+1} {n+1\choose q} 3^q (-1)^{n-q}
\left(\frac{z}{(1+z)^2}\right)^q
\; dz
\\ = - \frac{1}{2\pi i}
\int_{|z|=\epsilon}
\frac{(1+z)^{2n+2}}{z^{n+3}}
\left(\frac{3z}{(1+z)^2}-1\right)^{n+1}
\; dz
\\ = - \frac{1}{2\pi i}
\int_{|z|=\epsilon}
\frac{1}{z^{n+3}} (-1+z-z^2)^{n+1}
\; dz.$$
Put $w=-z$ which just rotates the small circle to get
$$\frac{1}{2\pi i}
\int_{|w|=\epsilon}
\frac{1}{(-w)^{n+3}} (-1-w-w^2)^{n+1}
\; dw
\\ = \frac{1}{2\pi i}
\int_{|w|=\epsilon}
\frac{1}{w^{n+3}} (1+w+w^2)^{n+1} \; dw.$$
We get for the final answer
$$[w^{n+2}] (1+w+w^2)^{n+1}$$
but we have $2n+2-n-2 = n$ and thus exploiting the symmetry
of $1+w+w^2$ we get
$$[w^n] (1+w+w^2)^{n+1}.$$
To evaluate the RHS introduce the integral representation
$${k\choose n-k} =
\frac{1}{2\pi i}
\int_{|z|=\epsilon}
\frac{(1+z)^k}{z^{n-k+1}} \; dz.$$
This gives for the sum the representation
$$\frac{1}{2\pi i}
\int_{|z|=\epsilon}
\frac{1}{z^{n+1}}
\sum_{k=0}^{n+1} {n+1\choose k} \left((1+z)z\right)^k \; dz
\\ = \frac{1}{2\pi i}
\int_{|z|=\epsilon}
\frac{1}{z^{n+1}} (1+z(1+z))^{n+1} \; dz
.$$
The answer is
$$[z^n] (1+z+z^2)^{n+1},$$
the same as the LHS, and we are done.
We have not made use of the properties of complex integrals here so
this computation can also be presented using just algebra of
generating functions.
This MSE link has another computation in the same spirit.
Apparently this method is due to Egorychev although some of it is
probably folklore.