If I interpret the request a bit differently, I would say that the Steenrod operations in the cohomology of a spectrum tell you about the attachments of the cells. If Sq1x=y, then a cell dual to y is attached by a map of degree 2 mod 4 to a cell dual to x. Similarly, Sq2x=y tells us the attaching map is η, Sq4 detects ν and Sq8 detects σ. This doesn't go very far, but may help with the need to 'get a real grip on what they're doing'.
Next, let's assume you're really interested in homotopy, not just (co)homology. A class dual to a homology class in the image of the Hurewicz homomorphism must be indecomposable under the action of the Steenrod algebra, by naturality w.r.t. the map Sn⟶X. This limits the homotopy of X which can be detected by the homomorpism π∗X⟶H∗X: the homomorphism H∗X⟶H∗Sn can only map indecomposables non-trivially, since all classes in degrees below n must go to 0.
Then there are the relations. The fact that Sqn is decomposable when n is not a power of two tells us that if y=Sqnx, there must be other classes between x and y. EG, Sq3x=y≠0 tells us that Sq2x≠0 also, since Sq3=Sq1Sq2. So our spectrum can't have just two cells, dual to x and y, but must have a three cell subquotient with top cell attached by 2 (mod 4) to a cell attached by η to the bottom cell.
Or, if Sq2Sq2x=y≠0 then we must also have nonzero classes Sq1x and Sq2Sq1x, since Sq2Sq2=Sq1Sq2Sq1, and vice versa, if Sq1Sq2Sq1x=y≠0 then Sq2x≠0 as well. This leads to an easy proof that the mod 2 Moore spectrum M isn't a ring spectrum, since 2π0M=0 but π2M=Z/4, by looking at the obstruction to attaching the top cell of a putative spectrum with nonzero cohomology spanned by x, Sq1x, Sq2Sq1x, and Sq1Sq2Sq1x. More, the fact that you can only add such a top cell if you also have a class Sq2x so that the top cell can be attached by the sum of Sq1 on Sq2Sq1x and Sq2 on Sq2x shows that η2 (corresponding to the path Sq2Sq2 from bottom to top, must lie in the Toda bracket ⟨2,η,2⟩, corresponding to the path Sq1, Sq2, Sq1 from bottom to top.
Similarly, y=Sq1Sq2x tells us that homotopy supported on a cell dual to x can be acted on by v1 to get y, literally if we have a ku-module and multiply by v1∈ku2, or as the Toda bracket ⟨2,η,−⟩ more generally. The key fact here is that v1∈ku2 is in ⟨2,η,1ku⟩, where 1ku:S⟶ku is the unit.
Likewise, Sq2Sq1Sq2x=y corresponds to multiplication by the generator of ko4, literally for ko-modules, or as a bracket ⟨η,2,η,−⟩ more generally. Here you have to be in a situation where 2ν=0 to form the bracket, since ⟨η,2,η⟩={2ν,6ν}. This hints that the role of ν is non-trivial in real K-theory, despite going to 0 under the homomorphism π∗S⟶π∗ko and despite the cohomology of ko being induced up from the subalgebra A(1) generated by Sq1 and Sq2. The Adem relation Sq2Sq1Sq2=Sq1Sq4+Sq4Sq1 shows that Sq4 must act nontrivially if Sq2Sq1Sq2 does. Also, the fact that A(1)//A(0) is spanned by 1, Sq2, Sq1Sq2, and Sq2Sq1Sq2 tells us (with a bit more work) that we can build HZ as a four cell ko-module.
A good way to organize all this information is the Adams spectral sequence, which tells you that the mod p cohomology of X gives a decent first approximation, ExtA(H∗X,Fp), to the homotopy of the p-completion of X.