As far as physical significance goes, I think its more relevant to talk about what the Riemann curvature tensor is in a frame-field, rather than in a coordinate basis.
For the Schwarzschild metric, we can set up a coframe basis
w1 = sqrt(1-r_s/r) dt
w2 = dr/sqrt(1-r_s/r)
w3 = r d\theta
w4 = r \sin \theta d\phi
The metric then becomes diagonal, equal to
ds^2 = -c^2 w1^2 + w2^2 + w3^2 + w4^2
With this metric, the dual of w1 is a unit vector in the t direction, usually written as \hat{t}, a "t" with a "hat" over it (the latex seems blurry).
Similarly the dual of w2 is a unit vector in the r direction, the dual of w3 a unit vector in the theta direction, and the dual of w4 a unit vector in the phi direction.
Then we can write
R^{2}{}_{121} = -\frac{r_s}{c^2\, r^3}
R^{3}{}_{131} = R^{4}{}_{141} = \frac{r_s}{2\, c^2\, r^3}
I've chosen the initial superscript to tie-in with the geodesic deviation equation, but I'm running out of time to explain the details thereof.
If we take the first step towards geometric units by making c=1, we can see that the units of the Riemann in the frame field are 1 / length^2, where "length" could be a space interval (say feet), or a time interval (say nanoseconds) as long as you choose units where c=1 (1 foot/ nanosecond works fairly well, though people don't use feet much in the literature for distance units! - and 1 foot per nanosecond is only approximately correct).
Note that the Riemann curvature has the same units as gaussian curvature, which can be defined as the the products of the two principal curvatures for a 3-d space
http://en.wikipedia.org/w/index.php?title=Gaussian_curvature&oldid=388108115
however, the gaussian curvature is a measure of curvature that's independent of any specific embedding , unlike the "principal curvature".
Sectional curvature is another interesting topic to read on that is closely related - unfortunately I don't use it very much. I'm pretty sure there is a nice way to explain how gaussian curvature, sectional curvature, and the Riemann curvature tensor all tie in together, but I only actually use the Riemann curvature personaly.