Technically no, although it depends on what you mean by "secure".
Usually, when using a HSM for a CA, we mean: the CA private key (usually RSA) is generated, stored and used within the HSM, and the HSM will commit honourable suicide rather than letting that key ever exit its entrails. Up to the tamper-resistance of the HSM and how bug-free its firmware is, this ensures that even if the host machine is fully hijacked by an attacker and/or the attacker has physical access to the CA machine, then the attacker will not obtain a copy of the private key. At best he will be able to use the HSM to generate arbitrary signatures, but if the HSM is physically recovered then the attacker can know longer use the private key.
YubiHSM does not do RSA or DSA or any other algorithm relevant to asymmetric cryptography. YubiHSM is symmetric only (AES...). Thus, if you used it for a CA private key, then it would have to be along these lines: the RSA private key would be stored encrypted, and the symmetric key stored in the YubiHSM. However, when the private key would have to be used, it would first be loaded and decrypted in the RAM of the host machine, and that machine would then use its CPU to generate the signature.
I am not aware of any existing driver (Windows CSP, PKCS#11 driver...) which would make the necessary glue, but, in any case, it would void much of the interest of using a "HSM" since it, by nature, allows the private key to live outside of the tamper-resistant hardware.
YubiHSM is meant to support things like one-time passwords, not X.509 certificate authorities. A cheap alternative to a full HSM would rather be a smart card: that kind of hardware includes cryptographic accelerators which allow for efficient generation, storage and usage of asymmetric key pairs.