We consider the problem of recovering a complete (i.e., square and invertible) matrix $\mathbf A_0$, from $\mathbf Y \in \mathbb{R}^{n \times p}$ with $\mathbf Y = \mathbf A_0 \mathbf X_0$, provided $\mathbf X_0$ is sufficiently sparse. This recovery problem is central to theoretical understanding of dictionary learning, which seeks a sparse representation for a collection of input signals and finds numerous applications in modern signal processing and machine learning. We give the first efficient algorithm that provably recovers $\mathbf A_0$ when $\mathbf X_0$ has $O(n)$ nonzeros per column, under suitable probability model for $\mathbf X_0$. In contrast, prior results based on efficient algorithms either only guarantee recovery when $\mathbf X_0$ has $O(\sqrt{n})$ zeros per column, or require multiple rounds of SDP relaxation to work when $\mathbf X_0$ has $O(n^{1-δ})$ nonzeros per column (for any constant $δ\in (0, 1)$). } Our algorithmic pipeline centers around solving a certain nonconvex optimization problem with a spherical constraint. In this paper, we provide a geometric characterization of the objective landscape. In particular, we show that the problem is highly structured: with high probability, (1) there are no "spurious" local minimizers; and (2) around all saddle points the objective has a negative directional curvature. This distinctive structure makes the problem amenable to efficient optimization algorithms. In a companion paper (arXiv:1511.04777), we design a second-order trust-region algorithm over the sphere that provably converges to a local minimizer from arbitrary initializations, despite the presence of saddle points.